Research on aerosol sources and chemical composition: Past, current and emerging issues

This article appeared in a journal published by Elsevier The attachedcopy is furnished to the author for internal non-commercial researchand education use including for instruction at the authors institution

and sharing with colleagues

Other uses including reproduction and distribution or selling orlicensing copies or posting to personal institutional or third party

websites are prohibited

In most cases authors are permitted to post their version of thearticle (eg in Word or Tex form) to their personal website orinstitutional repository Authors requiring further information

regarding Elsevierrsquos archiving and manuscript policies areencouraged to visit

httpwwwelseviercomcopyright

Authors personal copy

Research on aerosol sources and chemical composition Past current andemerging issues

AI Calvo a C Alves a A Castro b V Pont c AM Vicente a R Fraile b

a Centre for Environmental and Marine Studies (CESAM) University of Aveiro 3810-193 Aveiro Portugalb Department of Physics IMARENAB University of Leoacuten 24071 Leoacuten Spainc Laboratoire dAeacuterologieOMP UMR 5560 Universiteacute de Toulouse III CNRS-UPS 14 av E Belin 31400 Toulouse France

a r t i c l e i n f o a b s t r a c t

Article historyReceived 23 April 2012Received in revised form 12 September 2012Accepted 15 September 2012

In spite of considerable progresses in recent years a quantitative and predictive understanding ofatmospheric aerosol sources chemical composition transformation processes and environmentaleffects is still rather limited and therefore represents a major research challenge in atmosphericscience This review begins with a historical perspective on the scientific questions regardingatmospheric aerosols over the past centuries followed by a description of the distributionsources transformation processes and chemical and physical properties as they are currentlyunderstood The major open questions and suggestions for future research priorities are outlinedto narrow the gap between the present understanding of the contribution of both anthropogenicand biogenic aerosols to radiative forcing resulting from the spatial non-uniformity intermittencyof sources unresolved composition and reactivity

copy 2012 Elsevier BV All rights reserved

KeywordsAerosolsHistorical aspectsChemical compositionSourcesResearch perspectives

Contents

1 Introduction and scope of the review 02 History of aerosol science 03 Aerosol chemical composition main sources 0

31 Main aerosol sources 0311 Anthropogenic sources 0312 Natural sources 0

32 The chemical composition of aerosols 0321 Sulphur species 0322 Nitrogen species 0323 Carbonaceous species 0

4 Suggestions for further research 05 Concluding remarks 0Acknowledgments 0Appendix A Supplementary data 0References 0

1 Introduction and scope of the review

Today there is a growing interest in improving air qualityby both the general public and individual governments This

Atmospheric Research 120ndash121 (2013) 1ndash28

Corresponding authorE-mail address anacalvouapt (AI Calvo)

0169-8095$ ndash see front matter copy 2012 Elsevier BV All rights reservedhttpdxdoiorg101016jatmosres201209021

Contents lists available at SciVerse ScienceDirect

Atmospheric Research

j ourna l homepage wwwe lsev ie r com locate atmos


interest has prompted an important increase in atmosphericpollution research which is a complex task requiring knowl-edge of all the factors and processes involved the emission ofpollutants to the atmosphere by natural andor anthropogenicsources the transport the chemical and physical transforma-tions and deposition of the pollutants (dry and wet) andfinally their effects on living beings All these processes mustbe considered from different perspectives and at several scalesboth spatial (molecular micro-scale meso-scale continentaland global) and temporal (from less than one second to years)

Among the numerous atmospheric pollutants (NOx SOxCO VOCs ndashvolatile organic compoundsndash PAHs ndashpolycyclicaromatic hydrocarbonsndash etc) aerosols are of particularinterest In the language of atmospheric sciences the termlsquoaerosolrsquo a word derived from aero (Greek ἀήρἀέρος air) andsolution (solutio -onis solution) designates the solid andorliquid particles in suspension in an air mass excluding cloudsand rain droplets (or crystals) (Meacuteszaacuteros 1999) moregenerally defined with the term of hydrometeors The naturaland anthropogenic sources releasing primary particulatematter to the atmosphere are many and varied and thesesources determine the physical characteristics of aerosols (sizedensity surface etc) and their chemical composition As aresult of this wide range of possible primary sources and of thevarious formation mechanisms of secondary aerosols particu-late matter (PM) is a combination of particles of differentorigins composition and granulometric distribution

The size number and chemical composition of the particlesmay vary due to a number of processes (Delmas et al 2005)nucleation (homogeneous and heterogeneous) coagulationand adsorptiondesorption After their release and evolutionthe particlesmay be removed from the atmosphere by dry andor wet deposition and heterogeneous chemistry (in-cloudscavenging or below-cloud scavenging)

The size of a particle may range from a few nanometers toseveral tens of microns Size is the main parameter forcharacterising aerosol behaviour Most aerosol characteristicsas well as the processes governing these characteristics andtheir impacts depend on particle size (EPA 1996 Seinfeld andPandis 1998) Today the lognormal function is the mostwidely used system for describing size distributions (Castroet al 2010) However the only reason for using it is the goodfit shown in awide range of empirical data Other distributionssuch as themodified gamma distribution (Calvo et al 2011) orWeibull distribution (Brown and Wohletz 1995) have alsobeen used to characterise atmospheric aerosols In generalambient particle distribution corresponds to the sum of mlognormal distributions

Moreover chemicalmicrophysical and optical properties ofaerosols govern a number of impacts including health(Schleicher et al 2011) climate (Das and Jayaraman 2012)acid rain (Zhang et al 2012) ecosystems (Katul et al 2011)visibility (Yuan et al 2006) and buildingmaterials (Costa et al2009)

Because of the many and varied domains that concernparticulate matter it is necessary to control aerosol concentra-tions and establish thresholds especially to protect humanhealth and the environment in general Thus maximumstandards have been set by many governments in the worldIn the case of Europe the current regulation 200850CEincluded for the first time the control of the fraction PM25

(particles with aerodynamic diameterb25 μm) because of itseffects on health The threshold value of 20 μg mminus3 must beattained by the 1st of January 2020 It seems obvious that weneed to know in detail everything related to aerosols (sourcescomposition size transport processes interactions etc) Thisknowledge enables us to device a number of control strategiesto reduce aerosol emissions and minimise their impact alsoreducing the emission of precursor gases

Aerosol science has seen a huge progress from its beginningin the second half of the 20th century Many scientists havecontributed to advances in this discipline These contributionsand the important technological developments in recent de-cades have resulted in the deep knowledge that we have todayof aerosols In particular tools such as modelling exercises orsatellite observations integrate spatially and temporally aerosolproperties and contribute largely to the knowledge of impactsand feedbacks at large spatial and temporal scales

It is certainly a valuable resource to compile in one singlepiece of work all the information included in the studies carriedout in the past few years to illustrate the evolution of aerosolscience and provide the scientific community with a widebibliography that may be helpful in current investigations andfor opening new research lines Some overviews have focusedon the evolution of the equipment used to measure aerosols(Spurny 1998 McMurry 2000b Spurny 2001) on theemissions from biomass burning (Koppmann et al 2005 Reidet al 2005a 2005b) on organic atmospheric aerosols(Jacobson et al 2000 Hoyle et al 2011) on carbonaceousaerosols (Pio et al 2011) on satellite remote sensing ofaerosols (Li et al 2009Mishchenko 2010) on aerosol impacts(Lohmann and Feichter 2005 Levin and Cotton 2008Mahowald et al 2011b) on atmospheric composition change(Monks et al 2009) on natural aerosol interactions andfeedbacks (Carslaw et al 2010) on aerosolndashcloud interaction(Flossmann and Wobrock 2010) on stratospheric aerosols(Deshler 2008) or on aerosol models (Holmes and Morawska2006) This study includes a survey of literature illustrating thecurrent state-of-the-art in a number of aerosol topics mainlysources and in situ chemical composition focusing on organiccompounds This paper also outlines the main aspects deter-mining current aerosol research and future perspectives

2 History of aerosol science

Aerosol studies have been recognised as a science from theend of World War II Many scientists from a wide range ofdifferent research fields (meteorology physics engineeringchemistry mathematics etc) have contributed to the founda-tion and evolution of aerosol science Besides we must notforget the importance of the technological progress and thepolitical and economic events which have promoted thisscience in one way or another (Spurny 2001)

Aerosol history is closely linked to the history of atmo-spheric pollution The existence of unpleasant and harmfulparticleswas already recorded by theRomans who complainedabout dirty air in ancient Rome In 1273 coal burning wasforbidden in London because of high concentrations ofparticulate matter A Royal Decree was issued by Edward I in1306 Later during the reigns of Richard II (1307ndash1377) andHenry V (1377ndash1422) several regulations were issued anddifferent taxes were imposed with the aim of restricting coal

2 AI Calvo et al Atmospheric Research 120ndash121 (2013) 1ndash28


burning in the city of London In France in 1382 king CharlesVI banned the emission of ldquonauseating fumesrdquo in Paris In1661 John Evelyn presented Charles II with the pamphletFumifugium the first document dealing with atmosphericpollution by particulate matter This pamphlet includes adescription of pollution in the city of London (Lodge et al1969) From the 16th century and until the mid-20th centurythe emissions resulting from coal burning (gradually replacingwood)were themain focus in atmospheric pollution studies InLondon despite the regulations mentioned above the problemof the fumes persisted and there is written evidence of sulphurfog events in documents from the 18th century The situationdeteriorated so much that at the beginning of the 19th centurythe English parliament formed a committee to issue measuresto mitigate the problem (Brimblecombe 1998) In 1775 cancerwas related for the first time to the presence of lsquosubstancesrsquo inthe working place as a result of the high incidence of thisdisease among young boys employed as chimney sweeps inEngland (Finlayson-Pitts and Pitts 1986)

The scientific interest in atmospheric aerosols began in the18th century during the Enlightenment a time when thenatural sciences in general were rapidly developing A numberof theories appeared in this period dealing mainly with theorigin of particulate matter and its effects in the atmosphere Atthe end of the 19th century Udden (1896) describes the studiesof several geologists relating soil formation and atmosphericaerosols Simultaneously meteorologists recognise the impor-tant influence of aerosols on the formation of precipitation onatmospheric visibility and on the thermal and radiative balance(Husar 2000) The doctoral dissertation by Kempf (1914)represents amilestone in the discipline theorising on the originof aerosols and listing all the scientific literature on the topicuntil 1870 Kempf groups the emitting sources into 5 categories(i) terrestrial gas emissions (ii) electricity (iii) dust cloudsfrom meteorites (iv) volcanic emissions (v) wind-transporteddust clouds and (vi) combustion processes (Alves 2001)

The scientific methods for establishing the causes and originof atmospheric aerosols were outlined by Egen (1835)According to this author the causes may be identified by(1) direct observation for example of smoke haze (2) smell ofthe air (3) temporal variation (4) decay with the distancefrom the source (5) variations of the concentration with winddirection or (6) air mass trajectory analyses Themethodologyproposed by Egen is virtually the same as the one used incurrent atmospheric sciences based on a sourcendashreceptorrelationship

The local dispersion of atmospheric aerosols and thetransport over long distances is from early times a matter ofscientific discussion According to Kempf (1914) the firstreport on a transboundary tropospheric transport event waswritten by Sir Francis Bacon around 1600 This noblemanreports the complaints which the Gasgogners a wealthy familyfrom the South of France presented to the English monarchafter the nasty smoke from the burning of algae in Sussexarrived during the vine flowering period endangering theharvest of that year

In 1767 Wargentin claimed that forest fires in Russia andFinland caused the hazes and mists observed in Central Europeand considered the possibility of mapping the dispersion ofsmoke taking into account both wind intensity and direction(Alves 2001)

From the end of the 18th century to the mid-19th centurythe plains to the North of the Alps in a region extending fromParis to Warsaw were frequently covered by a thick haze layerthat motivated several studies about the possible causestransport and effects The origin of this atmospheric phenom-enon was attributed to the peat burning resulting from thedrainage of marshland to obtain new agricultural areas in theNW of Germany and in the Netherlands It was not until 1870that these burnings and the resulting atmospheric problemsended (Prestel 1861)

According to Danckelman (1884) the hazes and smokesfrom burnings in the African savannah observed in differentregions of Europe are known since Roman times It is importantto mention a study by Dinkage (1891) about the spreading intime and space of dust clouds from the Sahara

According to Husar (2000) the first mass balance with thechemical composition of aerosol was carried out by Barac in1901

The studies by Rafinesque (1819 1820) on the atmosphericbehaviour of aerosols theorised for the first time on theprocesses for removing particulate matter from the atmo-sphere including the mechanisms of dry and wet depositionThis author was a pioneer in recognising that ldquopart of theatmospheric aerosols is chemically formed of a combinationof gases and elementary particles dissolved in the airrdquo Theexperimental verification of these theories about the formationof secondary aerosols was carried out some 80 years later

On the other hand atmospheric phenomena also revealedthe presence of particulate matter and the interaction withradiation As early as in the 18th century we find studiesdealingwith this type of phenomena (Franklin 1784) Kiessling(1888) attributed the ldquored sunsetrdquo to the stratospheric aerosolsemitted during the Krakatoa eruption in Indonesia

Spurny (2001) distinguishes two periods in the researchand development of the methodology for measuring aerosolsthe pre-classical period (before 1900) and the classical periodThe first efforts in aerosol science are closely related to theinitial development of colloidal chemistry (Spurny 1998)After the experiments by Espy in 1841 (McMurry 2000a) andH Becquerel in 1847 (Podzimek and Cartens 1985 Podzimek1989) on the existence of fine particles in the air ndash known todayas condensation nuclei or CN ndash Coulier (1875) was the firstauthor to publish a study demonstrating that when the airexpands adiabatically condensation occurs more easily innon-filtered air than in filtered air Later from 1880 on Aitkenconfirmed Couliers hypothesis (Aitken 1890) on CN and theirimportance in cloud formation (Spurny 2001)

The first existing record of aerosols being generated inlaboratory conditions is the one described by Leonardo daVinci(Kerker 1997) in the Codex (15061509) Several hundredyears later in 1866 John Tyndall repeated da Vincis experi-ments and was the first author to apply this method to thedetection of atmospheric particulate matter indoors (Tyndall1871 Gentry 1997)

The use and development of experimental measurementtechniques are themain features of the classical period in aerosolphysics (Spurny 1993) which lasted until themid-20th centuryand finished with the publication of The Mechanics of Aerosols(Fuchs 1964) The term aerosol was coined in this period in1918 by the physicist and chemist EG Donnan Later in 1920the term was introduced in the literature on meteorology by A

3AI Calvo et al Atmospheric Research 120ndash121 (2013) 1ndash28


Schmauss the director of the Central Meteorological Station inMunich Germany (Schmauss 1920a 1920b)

A few measurements of microbiological particles werecarried out indoors before 1900 (Preining 1996 Sigerson1870) However the main progress in the methods or in-struments of measuring aerosols took place later mainly after1920 Examples of some of the first books published onatmospheric particulate matter are De re metallica (Agricola1912) Smoke a study of town air (Cohen and Ruston 1932)Industrial dust (Drinker and Hatch 1936) Les Aeacuterosols (Avy1956) andAerosol Science (Davies 1966) Thenegative effects ofdust and industrial aerosols on human health were alsodescribed in this period (Sinclair 1950) The growing incidenceof conditions such as silicosis in the industry and in miningresulted in the development of techniques for measuring dustin the workplace (Drinker and Hatch 1954) In the 1920s silicawas identified as the cause of a number of lung problemsin particular pneumoconiosis and silicosis (Collins 1926)Walton and Vincent (1998) provide an overview of the evo-lution of aerosol measurement instrumentation in occupationalhygiene

Up to the mid-1920s the principal method of samplingaerosols was the sugar tube (Walton 1982 Spurny 2001) Thisdevice comprised a 32 mm diameter tube filled to a depth ofabout 100 mm with 10ndash20 mesh sugar granules Air wasdrawn through the granules by a hand operated pump and thecollected dust was analysed by dissolving the sugar andfiltering the residue which was then weighed to provide anestimate of the airborne mass As well as being difficult to usethis method was criticised because reductions in themeasureddust concentration in mines and other dusty environmentswere not matched by corresponding falls in dust relateddiseases (Cherrie and Aitken 1999)

Current measurement methods make use of all thetechnical progress made after the 1960s Spurny (19982000 2001) and McMurry (2000b) provide good reviews ofthe various aerosol measurement methods Flagan (1998)describes the history of the electrical devices to measureaerosols from the early efforts to understand the nature ofatmospheric electricity and the associated charge transferuntil the development of the instrumentation currentlyavailable to measure particle sizes

Important innovations have been developed in the in-strumentation used for sampling as well as in the devicesand techniques employed in laboratory analyses (McMurry2000b) Particularly relevant are the improvements in cascadeimpactors and in electric mobility analysers Huge progress hasalso been made in optical particle counters The developmentsin the field of aerosol chemistry have been equally successfulInnovative and highly sensitive techniques (chromatographymass spectrometry laser and plasma spectroscopy X-rayspectrometry etc) enable us now to identify in one particularsample a wide range of organic and inorganic components Inaddition the application of a number of modern analyticaltechniques has prompted the development of the disciplineinvolved in measuring aerosols and identifying their chemicalcomposition Despite this progress each analytical techniquenot only has advantages but also drawbacks andmanydifferenttechniques must be applied onto one particular sample toobtain an accurate description of the chemical composition ofaerosols Finally microscopy has improved our knowledge of

the individual chemical composition the morphological char-acteristics and the interactions of particles (Coz et al 2010)

Parallel to the progress made in sampling and analyticaltechniques modelling has become a valuable tool in the studyof aspects such as formation growth processes sourceapportionment and the transport of atmospheric aerosols aswell as their impacts (eg Gong et al 2006 Koch et al 2011Wang et al 2011a Yu 2011)

Furthermore the optical characteristics of aerosols arecurrently becoming a topic of interest By means of a radiativetransfer code the measurements determine the radiativeimpacts associated with the presence of aerosols thusincreasing our knowledge of regional or global climatevariations on a large time scale One current issue of specialinterest is the impact of black carbon (BC) sometimes referredas elemental carbon (EC) on cloud condensation nuclei (CCN)or on the evolution of snow layers (Skeie et al 2011) Similarlythe characterisation of the fractions of organic matter that canalso absorb solar radiation efficiently known as brown carbonand their contribution to aerosol light absorption and radiativeforcing is a current topic of interest (Park et al 2010 andreferences therein)

The important increase in the number of publicationscontaining the word ldquoaerosolsrdquo (httpwwwsciencedirectcom) clearly illustrates the development of aerosol scienceand the growing interest of the scientific community Thenumber of publications has soared from nearly 16800 in the1980s to over 53500 in the first decade of the 21st century Ifthe articles including both ldquoaerosolsrdquo and ldquosourcesrdquo areconsidered the increase is also clear growing from 8800publications in the 1980s to over 33700 between 2000 and2010 A maximum was reached in 2011 with nearly 4880publications

3 Aerosol chemical composition main sources

31 Main aerosol sources

Depending on their origin aerosols may be natural oranthropogenic The main sources of anthropogenic particulatematter in the atmosphere lie in urban and industrial areas andwe may mention here traffic (exhaust emissions road surfaceabrasion brake and tyre wear particle resuspension frompaved roadways) different industrial activities (emissions frompower plants oil refineries mining) building (excavations soilmovement demolitions) and emissions from housing (heatingfood cooking) In rural areas on the other hand the mainsources of aerosols are biomass burning and the emissions dueto various farming activities

Among the natural sources of particulate matter we maymention the seas and oceans deserts soil volcanoes vegeta-tion wildfires and lightning This wide range of sourcesgenerates particles with very different chemical compositionscommonly related to their origin

The project ECCAD (Emissions of atmospheric CompoundsCompilation of Ancillary Data httpmunkipsljussieufr) pro-vides the scientific community with a number of digital mapsand data series useful to quantify the surface emissions ofatmospheric chemical components from various sources(ocean fires vegetation etc) This project gathers data onmany chemical species including several components of



aerosols and of their precursor gases These ancillary data foremissions will implement the existing inventories with thedata required for the interactive computation of the emissionsby means of relatively simple algorithms or complete modelssimulating emissions Authors such as Andreae and Rosenfeld(2008) have reviewed several studies and obtained estimationon particle emissionproduction and burdens for differentaerosol sources at global level

Table 1 summarises the main organic aerosol constituentsand sources Inorganic marker elements associated withvarious emission sources or processes have been included inTable 2 In cases where trace metals are released by more thanone technogenic process it can be useful to use element ratiosFor example CuSb values in particles released from traffic

brake wear are significantly higher than those of wasteincineration fly-ash samples Likewise certain industrialprocesses and the use of catalytic converters in road trafficresult in atmospheric fractionation of lanthanoid elements (Lato Lu) leading to distinctive anthropogenic geochemicalanomalies because these elements are rarely fractionated bynatural geological processes Thus aerosols emitted from oilrefineries using La-rich zeolitic fluid catalytic converters (FCC)or from power stations burning oils previously contaminatedby FCC will present LaCe values noticeably higher than the 05typical of most crustal materials On the other hand unchar-acteristically low LaCe values are typical of ceramic worksusing Ce as a pigment Also vehicle tailpipe particles derivedfrom the thermal and mechanical wear of catalytic converters

Table 1Main organic aerosol constituents and sources

Primary Secondary

Fossil fuelcombustion(eg vehicles)

Otheranthropogenicprocesses (egmanufacturingcooking)

Biogenic (egvascular waxes)and bioparticles(eg spores)

Biomassburning

Soil Gas-particlepartition(adsorption andabsorption)

Reactivecondensation(eg acidcatalysedreactions)

In-cloudprocessing

Alkanes alkenes alkanalsalkanoic acids diacids

Aromatics PAHs Hopanes steranes unresolvedcomplex mixture (UCM)

Photochemical products (eg carbonylsmethyl tetrols carboxylic acidsorganosulphates)

Sugars polyols polysaccharides

Levoglucosan

HULIS

Table 2Inorganic marker elements associated with various emission sources or processes

Secondary aerosols SO42minus NO3

minus NH4+

Sea salt Cl Na Na+ Clminus Br I Mg and Mg2+

Crustal or geological tracers Elements associatedwith feldspars quartz micas and their weatheringproducts (mostly clay minerals) ie Si Al K Na Ca Fe and associatedtrace elements such as Ba Sr Rb and Li In addition there will beaccessory silicates (notably zircon titanite and epidote) and repre-sentatives from the minority non-silicate mineral groups namelycarbonates sulphates oxides hydroxides and phosphates

Technogenic tracers Steel industry Cr Ni and MoCopper metallurgy Cu and AsCeramic industries Ce Zr and PbHeavy industry (refinery coal mine power stations) Ti V Cr Co Ni Zn As and SbPetrochemical industry Ni and VOil burning V Ni Mn Fe Cr As S and SO4

2minus

Coal burning Al Sc Se Co As Ti Th S Pb and SbIron and steel industries Mn Cr Fe Zn W and RbNon-ferrous metal industries Zn Cu As Sb Pb and AlCement industry CaRefuse incineration K Zn Pb and SbBiomass burning K and BrFirework combustion K Pb Ba Sb and SrVehicle tailpipe Platinum group elements Ce Mo and ZnAutomobile gasoline Ce La Pt SO4

2minus and NO3minus

Automobile diesel S SO42minus and NO3

minus

Mechanical abrasion of tyres ZnMechanical abrasion of brakes Ba Cu and Sb



show similar extremely low LaCe valueswhich can differ fromcrustal ratios by over 200 times (Moreno et al 2009)

311 Anthropogenic sources

3111 Traffic The concentrations of particles released bytraffic and their composition have been the object of studyfor many authors (eg Fang et al 2006 Martuzevicius et al2008) and still are a current topic under investigation Roadtraffic especially in urban areas is the main source ofprimary and secondary anthropogenic aerosols These parti-cles vary greatly in size and chemical composition dependingon the mechanisms involved in their formation Roadvehicles release through their exhaust pipes a mixture ofgases and ultrafine primary carbon particles (Jiang et al2005) Non-exhaust emissions from road vehicles includeparticles from brake wear tyre wear road surface abrasionand resuspension in the wake of passing traffic (Thorpe andHarrison 2008) Brake and tyre wear for example releases tothe atmosphere particles with traces of elements such asstrontium copper molybdenum barium cadmium chromi-um manganese and iron (EC 2004) Garg et al (2000) haveperformed brake dynamometer tests on 7 brake types widelyused in the US vehicle fleet Sanders et al (2003) and Iijimaet al (2007) have carried out similar experiments on brakelining materials considered to account for most of the for-mulations used in Sweden and Japan respectively Tyre wearan important contributor of PM10 emissions causes annuallosses of rubber from tyres in Europe of around severalthousands of tons (Thorpe and Harrison 2008) Because tyrescontain a vast array of both organic and inorganic constitu-ents research into the chemical composition of tyre rubberand wear debris is rather sparse (Rogge et al 1993)

Furthermore the ejection of particles from the pavement(Kupiainen et al 2004) and unpaved road shoulders(Moosmuumlller et al 1998) by resuspension processes must notbe forgotten (Bukowiecki et al 2010) Here we may mentionthe high number of particles registered in northern Europeduring the winter months when sand and salt are widely usedon roads to keep snow from freezing to ice (EC 2004) Usingdata from several European cities Querol et al (2004) haveshown that exhaust and non-exhaust sources contributeapproximately equal amounts to the total traffic-relatedemissions

Traffic is the main source of nitrogen oxides in urban areasand these act as the chemical precursors of nitrogen com-pounds (Singh and Sloan 2006) In addition road vehiclesrelease a wide range of metals in small concentrations amongothers copper zinc and cadmium (from tyres brakes andorwaste oil) (Hjortenkrans et al 2007) Traces of other elementssuch as potassium bromine or chlorine come from the motor(Pacyna 1998) Furthermore the vehicle catalytic convertersemit platinum palladium and rhodium (Prichard and Fisher2012) A drop in the atmospheric lead emissions from traffichas been registered as a result of the effective environmentallegislation (Napier et al 2008) Thus the sources and fluxes ofPb in the environment have significantly changed after the banof leaded gasoline worldwide (eg 1975 in the EEUU themid-1980s in Europe in 1997 in the large cities of China)(Zhang et al 2009b)

Trang andByeong-Kyu (2011) have shown that factors suchas traffic volume atmospheric dispersion from traffic rotariesfrequency of brake use vehicles coming to a complete stop andvehicle speed affect the contamination levels by heavy metals

Regarding ultrafine particle number emissions fromexhausts values between 2 and 70times1013 particles vehi-cleminus1 kmminus1 for light duty vehicles and between 20 and730times1013 particles vehicleminus1 kmminus1 for heavy duty vehicleshave been registered (Beddows and Harrison 2008 andreferences therein) For roadndashtyre interface emissions ultrafineparticles ranged between 37times1011 and 32times1012 particlesvehicleminus1 kmminus1 at speeds of 50 and 70 km hminus1 with meanparticle number diameters between 15 and 50 nm (Dahl et al2006) Brake-wear emissions are more difficult to measurebecause of their dependence on braking conditions (Sanderset al 2003)

PM emissions from diesel-powered vehicles are typically10ndash100 times higher than those from gasoline-poweredvehicles (Kittelson 1998) Special attention has been focusedon particulate matter from diesel engines due to its adversehealth effects it contains toxic chemicals including PAHswhich are known to cause damage to genetic material andare considered carcinogenic (Chirico et al 2010) In recentyears increasing attention has been focused on the use ofbiofuels (eg soybean-oil rapeseed-oil palm-biodiesel) asthey may have the potential to reduce air pollutant emissions(CO particle hydrocarbons PAHs PM) from diesel engines(Chien et al 2009) In general a drop in PM was registered aswell as a reduction in the particle mean diameter (Lin et al2007) Chien et al (2009) have shown that as the blendingpercentage of biodiesel increases the particles emitted shiftedto ultrafine and nanosize ranges They observed the same trendfor PAH emissions as they were highly related to PM

Gaffney and Marley (2009) offer an interesting review ofthe emissions from the combustion of the various fuels usedfor transportation

Besides cars emissions from other vehicles have also beenstudied (eg buses trucks tractors motorcycles) (Tsai et al2005 Cadle et al 2008 Tan and Tay 2008 Liu et al 2011)Important attention has also been focused on railway trafficemissions For example Lorenzo et al (2006) found that ironparticles predominate in emissions from railway linescontributing 29 μg mminus3 or 67 to the railway related PM10Aluminium and calcium particles contribute 23 and 10respectively The abrasion of the gravel bed and the re-suspension of mineral dust seem to be the main sources ofthese particles

On the other hand air traffic (Miracolo et al 2011) andmaritime traffic (Kim et al 2009) also contribute to theemissions of particulate matter or their precursors to theatmosphere Thus for example Barrett et al (2010) usedvalues of 138plusmn345 g NOx (as NO2) kgminus1 fuel 12plusmn04 g SOx

(as SO2) kgminus1 fuel 004 BC kgminus1 fuel and 002 organic carbon(OC) kgminus1 fuel in their study on globalmortality attributable toaircraft cruise emissions Moreover aircraft engines areemitters of metal particles (such as Al Ti Cr Fe Ni and Ba)(eg Starik 2008) Regarding ship emissions it is important totake into account their SO2 contribution 16 of the globalsulphur emissions (Corbett and Fischbeck 1997) and 54 ofthe total sulphate aerosol column burden over the Mediterra-nean in summer (Marmer and Langmann 2005) Ships also



release NOx (~70 g NOx kgminus1 of fuel burned) and carbona-ceous particulate matter (133 Gg yrminus1 or about 17 of thetotal global emissions) (Lack et al 2007 Gaffney and Marley2009)

3112 Industrial activities There is a wide range of industrialactivities emitting to the atmosphere particulate matter orgases that are precursors of particles Human activitiesgenerate between 60 and 80 of the sulphur emissions(Chuang et al 1997) Industrial pollution is characterised bythe large amounts of pollutants released in the various stages ofthe industrial processes and by the great variety of thesepollutants The type of pollutant dependsmainly on the type ofproduction process the technology and the rawmaterial used

Some of the activities generating more particle emissionsare the industries producing ceramics bricks and cementfoundries mining and quarrying all of which release largenumbers of primary aerosols either during the productionitself or during the manipulation and transport of the rawmaterials employed (Saacutenchez de la Campa et al 2010) Csavinaet al (2011) have studied emissions from mining operationsand the concentrations of toxic metals and metalloids such asAs Cd and Pb They found a bimodal distributionwithmeans ofaround 03 and 7 μm associated to a) smelting operations andb) wind erosion of mine tailings and fugitive emissionsrespectively Nickel vanadium manganese and copper arecommonly released in foundries (Pacyna 1998) Vanadiumand nickel are also released in the combustion of fuelndashoil in anumber of industrial processes (Jang et al 2007) Ahn and Lee(2006) found that Fe2O3 (396ndash745) and CaO (418ndash655)were the major constituents of particles from a steel plant andfrom a cement plant respectively On the other hand SiO2

(533ndash806) was the main constituent of the coal fly ash andthe foundry particles generated by a coal power plant and afoundry respectively Choeumll et al (2010) in their analysis of anepisode of industrial pollution plume found that steelworksare important point-source emitters of metallic pollutants (FeMn Zn) The authors highlighted the relevance of coagulationprocesses between industrial particles and particles from othersources as they found metal-rich particles internally mixedwith marine andor continental compounds

Energy production from fossil fuels is an important sourceof gases acting as precursors of secondary aerosols Coalburning in power plants generates primary particles formedby coal waste products such as clay sulphurs carbonateschlorides andmetalsmainlymercury and also by unburnt coalor char (Shindell and Faluvegi 2010)

Tohka and Karvosenoja (2006) carried out an importantstudy on fine particle emissions and emission reductionpotential in Finnish industrial processes Activities such as glasswool and fibre production nitric and sulphuric acid produc-tion non-ferrous metal production oil refineries sinteringplants coking plants lime production or mineral processinghave been included

Furthermore recycling plants and composting plantsrelease bacteria and fungi to the atmosphere (Domingo andNadal 2009)

3113 Coal burning Coal combustion mainly used to produceelectricity and heat constitutes another important source of

particulate matter and gaseous pollutants (Tsitouridou andAnatolaki 2007)

Focusing on residential coal combustion it constitutes aserious problemmainly in developing countries where limitedstudies have been carried out (eg Chen et al 2009 Shen et al2010) Factors such as coal maturity coal combustors orburning conditions influence the emissions from the combus-tion of this fossil fuel Toxic components such as PAHs or traceelements (eg As Se Hg Cr Cd Pb Sb Zn) (Liu et al 2008 Xuet al 2011) have been identified in coal combustion emissionsand usually they are present in the fine PM25 fraction (Linak etal 2007 and references therein) This fact makes them moredangerous for the human health (Liu et al 2008) In Chinaresidential coal combustion constitutes an important source ofair pollution (Li et al 2012b) contributing to 107 of thetotal PAHs emitted in 2004 (Shen et al 2010 Zhang et al2008) Emission factors of 16 EPA priority PAHs fromtested coals ranged from 625ndash116 mg kgminus1 (anthracite)to 253ndash170 mg kgminus1 (bituminous) with naphthalene andphenanthrene dominating in gaseous and particulatephases respectively (Shen et al 2010) Regarding BC andOC Chen et al (2009) carried out different combustion testsin three typical stoves for household burning of 13 coalsin honeycomb-coal-briquette and raw-coal-chunk formsThey found averaged BC emission factors (EFs) of 4 and7 mg kgminus1 for anthracite and 90 and 3050 mg kgminus1 forbituminous coal in briquette and chunk forms respectivelyEmission factors for organic carbon presented averagevalues of 60 and 100 mg kgminus1 for anthracite and 3740 and5500 mg kgminus1 for bituminous coal in both forms (briquetteand chunk) respectively Zhang (2005) obtained emissionfactors of 8820 mg kgminus1 for PM10 and 6860 mg kgminus1 forPM25 for residential coal combustion

Huang et al (2011) have compiled emission factors fromdifferent coal combustion sources An interesting review hasbeen provided by Xu et al (2011) including informationregarding aerosol ash formation during coal combustion

3114 Biomass burning Biomass burning is both a natural andan anthropogenic source of aerosols It includes the burning ofwoodland pastures and agricultural land after harvestingactivities to prepare the land for the next year (Ortiz de Zaacuterateet al 2005) Biomass burning is an important source of gasesand atmospheric particulate matter worldwide (eg 220ndash13500 Tg CO2 yrminus1 120ndash680 Tg CO yrminus1 ~38 Tg PM25 yrminus1)with a strong effect not only at the regional scale but also at sitesthousands of kilometres from the source (Ryu et al 2007McMeeking et al 2009 Alves et al 2011b)

Biomass burning emissions depend heavily on the combus-tion conditions which are broadly classified as flaming ndash inwhich a more complete oxidation is involved ndash and smoulder-ing (Koppmann et al 2005) A complete characterisation ofthese two phases is required when biomass burning emissionsare estimated

The aerosols generated by biomass burning consist mainlyof carbonaceous compounds (mainly OC and smaller amountsof EC) and lower concentrations of various inorganic compo-nents (Reid et al 2005b) This inorganic fraction is mainlyformed by insoluble dust and ashes The main constituents ofthe soluble salts are potassium ammonium sulphate andnitrate Considering the organic fraction 40ndash80 is water



soluble and an important percentage consists of acids (Reidet al 2005b Janhaumlll et al 2010) The elements that stand outare the ones resulting from the decomposition of cellulosesuch as levoglucosan used as a tracer of this type of aerosolinmany studies (Alves et al 2011a Oros et al 2006) RecentlyHolden et al (2011) have pointed out that probablylevoglucosan degradation during atmospheric aging of biomassburning emissions may likely result in an underestimation ofapportioned primary smoke contributions

Most of the particles emitted in biomass burning fall withinthe accumulation mode (Badarinath et al 2009) with a countmedian diameter of 100ndash150 nm A smaller coarse mode mdash

consisting of dust carbon aggregates ash and unburnt parts ofthe fuel (Formenti et al 2003 Hungershoefer et al 2008) andsometimes a nucleation mode are present (Radke et al 1991Janhaumlll et al 2010)

31141 Wildfires Wildfires destroy every year thou-sands of hectares with important losses in terms ofenvironmental damage economic disruptions and humanlives Aircraft satellite and ground-based measurementshave been carried out in order to characterise emissionsfrom forest fires (Cook et al 2007 Janhaumlll et al 2010Knobelspiesse et al 2011 Urbanski et al 2011) Among thenumerous parameters analysed is the attempt to estimateemission factors (g compound kgminus1 wood burnt) with the aimof understanding how fires influence and interact with theEarth system (van der Werf et al 2010) EFs have beenestimated in some laboratory studies (eg McMeeking et al2009) and in field campaigns (eg Alves et al 2010 2011a2011b) but many uncertainties persist Between 80 and 90of the particles generated by biomass burning has a diametersmaller than 1 μm (Alonso-Blanco et al 2012) Their charac-teristics vary greatly fromone fire to another depending on thetype of fuel the humidity the combustion phase (with orwithout flame) the wind conditions etc Moreover thephysical chemical and optical characteristics of these particleschange very fast as the smoke plume disperses making it morecomplicated to relate the characteristics of individual fires andthe group of smoke plumes affecting the radiative balance ofthe atmosphere (Reid et al 2005b Calvo et al 2010b)

31142 Domestic biomass burning An important fractionof all biomass combustion occurs in household stoves thatalthough of small scale are used in considerable numberhaving an important potential to contribute to atmosphericpollution especially in rural sites in Europe in winterEmissions from wood combustion are influenced by factorssuch as the stove design operating conditions combustionconditions and the species of wood and its characteristics(Johansson et al 2003) Important advances have been carriedout during the last years regarding the characterisation ofemissions from household stoves (Schmidl et al 2008Gonccedilalves et al 2010 Alves et al 2011b) Important dif-ferences have been registered between emissions fromfireplaces and those from othermore sophisticated equipmentThus fireplaces emit more particulate matter per kilogram ofwood burnt with a higher percentage of organic carbonHowever more sophisticated equipment (eg wood stoves)releases less aerosol mass concentrations with a higherpercentage of elemental carbon and inorganic compounds

31143 Agricultural burning The burning of agriculturalcrop residues in fields represents a regular part of the annual

agricultural activities of farmers worldwide and is consideredthe fourth most important type of global biomass burningwith estimations of around 500 Tg dm yrminus1 (dm drymatter) (Andreae and Merlet 2001 Bond et al 2004)although several authors have pointed out that theseemissions could be greatly underestimated (van der Werf etal 2010) At the same time crop residues are often used fordomestic heating and cooking mainly in developing coun-tries (Guoliang et al 2008)

Burning agricultural crop residues have a significant impacton greenhouse gas emissions and aerosol loading withimportant consequences at local and regional levels (van derWerf et al 2010 Calvo et al 2011) Ortiz de Zaacuterate et al(2000) have estimated that each kilogram of burnt dry cerealwaste releases around 1400 g of CO2 13 g of particulatematter(PM) and 19 g of NOx into the atmosphere

Koppmann et al (2005) and Reid et al (2005a 2005b)have listed the main characteristics of the particles generatedduring biomass burning including aspects such as the chemicalcomposition of aerosols their optical features size distribu-tions aging processes etc Furthermore Simoneit (2002) Orosand Simoneit (2001a 2001b) and Oros et al (2006) havepublished detailed reviews of organic compounds emittedfrom biomass burning Emission factors for species emittedfrom different types of biomass burning (tropical forestsavannah crop residues pasture maintenance boreal foresttemperate forest extratropical forest peatland chaparral opencooking patsari stoves charcoal burning and garbage burning)have been reported by Akagi et al (2011) These authorsinclude also a complete list of biomass loading combustionfactors and biomass consumption estimates for various fueltypes around the world

3115 Food cooking Another major source of fine particles inurban areas is food cooking Investigations of sources andchemical mass balance (CMB) calculations have shown thatthe emissions from meat charbroiling and frying account forabout 20 of all fine PM organic matter in Los Angeles(McDonald et al 2003) Robinson et al (2006) applyingCMB have attributed 320plusmn140 ngC mminus3 or 10 of theaverage ambient organic carbon to food cooking emissions inPittsburgh Pennsylvania More than 120 compounds werequantified when organic aerosols from meat cooking werestudied Palmitic stearic and oleic acids and cholesterol werethe most abundant (Mohr et al 2009) Some emission profileshave been obtained for US (Schauer et al 2001 McDonaldet al 2003) and Chinese (He et al 2004 Zhao et al 2006)cooking styles However emissions depend heavily on thecooking method cooking appliances and food ingredientsBuonanno et al (2009) found an important increase inemission factors associated with the increase in cookingtemperatures These factors not only affect the chemicalcomposition but also affect the aerosol characteristics ingeneral Thus regarding aerosol size distributions somestudies have reported a unimodal distribution ndash in theultrafinefine range (He et al 2004) ndash however a bimodaldistribution has been found in other studiesmdashwith an ultrafineand a coarse mode (Long et al 2000 Lai and Chen 2007)Rogge et al (1991) and Zhao et al (2006) have proposedseveral tracers of emissions from meat cooking from Westernstyle and Chinese cooking respectively The former includes



cholesterol myristic acid palmitic acid stearic acid oleic acidnonanal and lactones and the latter tetradecanoic acidhexadecanoic acid octadecanoic acid oleic acid levoglucosanmannosan galactosan nonanal and lactones

See and Balasubramanian (2008) studied the chemicalcharacteristics of PM25 emitted from different gas cookingmethods They concluded that the largest load of PM25 withthe highest number of chemical compounds was emittedduring deep-frying Pan-frying was the second largest emitterfollowed by stir-frying boiling and steaming Authors observeda higher organic pollutant concentration (OC PAHs and organicions) andmetals (mainly copper iron and zinc)when oil-basedmethods were used However more water soluble ionsinorganic ions such as fluoride chlorine and sulphate wereregistered when water-based cooking methods were appliedFurthermore a higher percentage of ultrafine particles(b50 nm) were registered when oil-based cooking methodswere used (69ndash90 of all particles during oil-based cooking55 during steaming and 62 during boiling) (See andBalasubramanian 2006) Sjaastad (2010) has studied exposureto fumes from Norwegian cooking styles during the pan fryingof beefsteak The author observed the presence of carcinogeniccomponents (higher aldehydes and PAHs) in fumes collected inthe breathing zone of the cook A higher exposure to somehazardous components was registered when frying on a gasstove than when frying on an electric stove Furthermore theauthor verified the importance of the choice of kitchenextraction hoods given that different types and settings ofkitchen extraction hoods involve different exposure conditionsAn important number of references about chemical composi-tion and aerosol size distribution from food cooking can befound in Sjaastad (2010)

3116 Garbage burning Garbage burning constitutes a sig-nificant emission source in both urban and rural areas Garbageburning is not included inmost inventories because it is usuallyillegal However a number of studies have shown that roughlyhalf of the garbage generated globally that is ~1000 Tg yrminus1may be burnt in open fires or incinerators (Christian et al2010) Thus a vast estimative could indicate that a total of500 Tg of C yrminus1 are injected into the atmosphere from thissource (considering that garbage is 50 C) (Forster et al 2007Mohr et al 2009)

Garbage is a heterogeneous fuel it contains not only a lot ofbiomass but also a lot of plastic paper and other materials suchas textiles rubberleather glass metal etc (Lemieux et al2000 and references therein Christian et al 2010) It has beenestimated that 12ndash40 of households in rural areas in the UScarry out the uncontrolled burning of garbage in their backyards(USEPA 2006) People mainly in rural areas burn garbage inbarrels (208 L drum ldquoburn barrelrdquo) underestimating theimportant health impact that these emissions may cause dueto the release of hazardous compounds such as dioxins(Costner 2006) Factors such as waste composition fullness ofthe barrel and combustion conditions contribute to determiningemissions (Lemieux et al 2000 2003)

Akagi et al (2011) based on Christian et al (2010)Lemieux et al (2000) USEPA (2006) and Yokelson et al(2011) have estimated emission factors for species emittedfrom garbage burning They have reported EFs of 98plusmn57 g kgminus1 065plusmn027 g kgminus1 and 527plusmn489 g kgminus1 for

PM25 BC and OC respectively Christian et al (2010) havepresented emission factors for individual particle speciesfrom garbage burning such as water soluble inorganic ionsmetals OC EC total carbon (TC=OC+EC) levoglucosanmannosan and galactosan They propose fine particle anti-mony (Sb) as garbage burning tracer and emphasise the factthat using levoglucosan and K as biomass burning tracers canbe inadequate in some areas since biomass burning andgarbage burning release similar concentrations of these twocompounds in the PM25 fraction

It is important to emphasise that HCl which is not usuallyobserved in biomass burning emissions (Lobert et al 1999)is registered in important concentrations in garbage burningemissions Christian et al (2010) found EFs (HCl) rangingbetween 165 and 98 g kgminus1 and significant additionalchlorine present in the particles (EFs for soluble Clminus aloneranged from 02 to 103 g kgndash1) These high EFs are linked tolarge amounts of polyvinyl chloride (PVC) (Lemieux et al2000 Akagi et al 2011)

A significant number of papers have focused on emissionsfrom waste incinerators and their impacts (Donnelly 1992Besombes et al 2001 Zeuthen et al 2007)

3117 Tobacco Tobacco constitutes another source of aero-sols affecting mainly indoor air quality (eg Edwards et al2001) Environmental tobacco smoke is a complex mixture ofgases and particles estimated to contain more than 4000individual chemical constituents Because of the presence ofcarcinogenic compounds (eg benzene aldehydes andbenzo(a)pyrene) linked to submicron particles aerosolsfrom tobacco smoke constitute a significant human healthrisk (Kleeman et al 1999) Numerous studies have beencarried out on tobacco aerosol size distribution chemicalcomposition and health impact (Chahine et al 2011 Pangand Lewis 2011 Talhout et al 2011) Several compoundshave been identified as specific tracers of environmentaltobacco smoke (iso- and anteiso-alkanes nicotine solanesol3-thenylpyridine gas phase nitrosamines or respirablesuspended particles) (Morrical and Zenobi 2002 andreferences therein) Hildemann et al (1991) have identifiedtobacco as a small source contributing organic fine particu-late matter to the outdoor urban atmosphere reporting thatcigarette smoke accounted for about 27 of the fine organicaerosol emissions in Los Angeles Rogge et al (1994) in theirstudy in the same city estimated that ambient fine cigarettesmoke particles were present at a concentration of 028ndash036 μg mminus3 accounting for 10ndash13 of the fine particle massconcentrations

3118 Fireworks Several studies have focused on fireworkevents and aerosol emissions (eg Barman et al 2008 Zhanget al 2010a Shi et al 2011) Fireworks though transientconstitute an important source of gases (ozone sulphurdioxide nitrogen oxides) (eg Ravindra et al 2003) andparticles (mainly metals ndash such as Sr K Ba Co Pb Cu ndash andorganic compounds) (Agus et al 2008 Moreno et al 2010)creating considerably short-term air pollution and serioushealth hazards (Witsaman et al 2006) The importanceof the role of coagulation processes has been observedcausing a significant reduction andor disappearance ofnucleation and small Aitken mode particles (Moumlnkkoumlnen et



al 2004 Agus et al 2008) during these events Zhang et al(2010a) determined a characteristic high particle density of27 g cmminus3 of the firework aerosols

312 Natural sources

3121 Mineral dust Among the natural primary particles wefind the mineral fraction commonly known as crustal fractionwhich is generatedmainly by the action of winds on the Earthssurface Mineral dust is one of the largest contributors to globalaerosol loading with important impacts associated (eg onradiative forcing providing nutrients to ecosystems affectingthe reflectivity of ice and snowor serving as CCNand ice nuclei)(DeMott et al 2010 Mahowald et al 2010 Zhang et al2010b) The size of dust aerosols is a crucial parameter whendust aerosol impacts are studied (eg Kok 2011b) RecentlyKok (2011a) has demonstrated that the size distribution ofnaturally emitted dust aerosols is independent of the windspeed at emission

The main sources are usually deserts dry lake beds andsemi-arid surfaces but any type of soil is a potential source ofthis type of aerosol Factors such as soil surface (texture androughness) soil moisture and vegetation cover as well aschanges in climatic parameters such as wind speed andprecipitation regulate the emission of mineral particles (Griniet al 2002 Washington and Todd 2005) This dependence ofdust production on soil and climate factors implies theexistence of feedbacks Thus some authors have pointed outa positive desertification feedback of mineral dust aerosol(Kluumlser and Holzer-Popp 2010)

The largest dust regions of the world lie within the globaldust belt Deserts such as the Sahara in the North of Africa thedeserts in the Arabian Peninsula and Oman Gobi andTaklimakan in China are part of this belt Other emittingregions lie outside this belt including Lake Eyre and the GreatArtesian Basin in Australia or desert areas in Patagonia and inWestern Argentina (Formenti et al 2011) At a global scale thedust regions in the northern hemisphere (mainly between 10degand 35deg) contribute more aerosols than the ones in thesouthern hemisphere (Prospero et al 2002 Formenti et al2011) The Sahara is the worlds major source of mineral dustand it has a strong influence in America and in Europe (Tafuroet al 2006 Calvo et al 2010a Thevenon et al 2011) Dustaerosols vary greatly in their characteristics from the opticalones to the microphysical ones

In general these particles are formed by calcite quartzdolomite clays (especially kaolinite and illite) feldspar andsmaller amounts of calcium sulphate and iron oxides amongothers (EC 2004 Klaver et al 2011) but the chemical andmineralogical compositions vary from one region to anotherdepending on the characteristics and the constitution of thesoil Fe in mineral dust has a special relevance due to its role inthe global biogeochemical cycling Iwamoto et al (2011) intheir study during an Asian dust event observed that iron fromdust particles could stimulate phytoplankton blooms

Because of the influence on marine ecosystem productiv-ity and radiative effects iron chemistry in mineral dust hasbeen the purpose of several studies (Balkanski et al 2007)On the other hand authors such as Ndour et al (2008) or ElZein and Bedjanian (2012) have recently discussed the

importance of TiO2 because it is involved in heterogeneousphotoreactions

The most important mechanisms for producing small dustaerosols are saltation (layer of soil moving with the wind justabove the surface) and sandblasting (release of dust aerosolduring impacts from saltating particles) (Shao et al 1993Grini et al 2002)

Authors such as Mahowald et al (2010) and Mulitza et al(2010) have estimated a doubling in dust over the past100 years Anthropogenic activity has contributed notorious-ly to this increase (Derbyshire 2007) Tegen et al (2004)have estimated annual dust emissions of 1921 Tg yrminus1 withan atmospheric turnover time of 52 days and an atmosphericburden of 166 Tg It has been estimated that between 7 and20 of these emissions have a diameter lower than 1 μm(Cakmur et al 2006) Submicron particles predominate inthe number size distribution of aerosol dust (Dusek et al2006) and the mass size distribution appears dominated bysupermicron particles (Trochkine et al 2003) Mahowaldet al (2011a) studied the interactions between desert dustand anthropogenic aerosols

Particles with diameters smaller than 100 μm may beairborne (Warneck 1988) Consequently when the windreaches a certain threshold speed mineral dust rises from theground to the atmosphere The particles closer to 100 μmhave more mass and remain for shorter periods in theatmosphere But smaller particles disappear through othermechanisms (especially joining larger particles) finally theparticles between 01 μm and 5 μm are the ones that remainfor longer in the atmosphere travelling up to 500 km in thecase of desert aerosol (Vergaz 2001)

It is important to take into account that although mineraldust has mainly a natural origin a minor load is emitted bydifferent anthropogenic sources such as dust emissions fromroads factories farming herding livestock and miningactivities (Ginoux et al 2010)

Recently an interesting paper on the physico-chemicalproperties of mineral dust from Africa and Asia has beenpublished by Formenti et al (2011)

3122 Sea spray aerosols Marine aerosol is the mostimportant aerosol fraction worldwide (White 2008) Mostmarine aerosols are primary but on the surface of seas andoceans we may find phytoplankton emitting various organiccompounds including dimethyl-sulfide (DMS CH3SCH3)which is considered one of the most significant precursors ofatmospheric sulphates in oceanic regions (Meacuteszaacuteros 1999Yang et al 2011) Marine salt is formed mainly by sodium andchloride with smaller amounts of other components such assulphate potassium magnesium and calcium The ocean is themain source of atmospheric sodium and chloride in coastalareas (Claeys et al 2010) Part of the chloride in the fineparticles of NaCl changes into a gaseous state in atmosphericreactions with sulphuric acid (in gaseous or aqueous phase)and nitric acid (in gaseous phase) (White 2008)

NaClethsTHORN thorn HNO3ethgTHORNrarrHClethgTHORN thorn NaNO3ethsTHORN

2NaClethsTHORN thorn H2SO4ethg thorn aqTHORNrarr2HClethgTHORN thorn Na2SO4ethsTHORN



This disappearance of chloride makes sodium the maintracer for particulate matter in marine salt (White 2008)

Primary marine aerosols are formed by the eruption ofrising bubbles through the sea-surface microlayer (SML) (Ryuet al 2007) The number of marine particles in the thresholdlayer over the ocean is directly proportional to the wind speed(Poacutesfai andMolnaacuter 2000) One single air bubble breaking up inthe ocean may produce up to 10 particles of marine aerosol(with diameters between 2 and 4 μm) These particlesmay riseuntil up to 15 cm above the surface and are known as jet dropsThe same single bubble may also produce several hundredparticles with diameters smaller than 1 μm (film drops)(Woodcock 1972) These drops are ejected to high altitudeswhere the water vapour evaporates (although not completely)because of the lower relative humidity By then the drop hasalready lost three fourths of its diameter (Warneck 1988) Therelative importance of primary marine aerosols has beenunderestimated both as a site of adverse biological effectsand as a medium for the transfer of energy and materialbetween seawater and the atmosphere

Marine aerosol generally contributes to the coarse fraction(Alves et al 2007b) but authors like Meacuteszaacuteros and Vissy(1974) have found smaller marine particles (005 μm) Thesubmicron fraction is of particular interest because of its directand indirect impacts on radiative transfer (Quinn et al 2002)

Marine aerosol can be found not only in coastal areas butalso at relatively high altitudes inland demonstrating along-range transport of this type of aerosol (Poacutesfai andMolnaacuter 2000)

In recent years the role of organic aerosols in the marineenvironment has received growing attention (Shank et al2012) For example Vignati et al (2010) present the results ofdifferent authors about global marine OC emissions They haveestimated that the global emission in the sub-micron size rangeof organic matter by sea spray processes is 82 Tg yrminus1compared to 24 Tg fine yrminus1 sea-salt emissions Globalmodelsunderpredict the OC especially during periods of planktonblooms when levels are underestimated by a factor of 5ndash20(ODowd et al 2008) OC correlates well with back-trajectoryweighted chlorophyll suggesting an oceanic OC source drivenby biological activity Different model estimates of the globalannual flux of marine OC have provided contradictory results(ODowd et al 2008 Roelofs 2008) but a general consensuswas reached this emission is comparable (or higher) inmagnitude to the fossil fuel OC source and increases thesimulated global OC burden by at least 20

Surfactants seem to be responsible for the enrichment ofmicrofloatable components in marine aerosol (McMurdoet al 2008)

3123 Biogenic emissions The biomass is responsible forthe emission of large amounts of gases and particles Thevegetation and some types of microorganisms contribute toprimary and secondary aerosol formation

Primary biogenic aerosols (PBA) emitted directly from thebiosphere to the atmosphere include pollen fern sporesfungal spores and other large particles with diameters of upto 100 μm With diameters smaller than 10 μm we find smallfragments and excretions from plants animals bacteriaviruses carbohydrates proteins waxes ions etc (Poumlschl2005 Winiwarter et al 2009) These aerosols are transported

over long distances and to high altitudes (up to 80 km)(Wainwright et al 2003 Prospero et al 2005) PBA globalemission has been estimated to range between 56 Tg yrminus1

(Db25 μm) (Penner 1995) and 1000 Tg yrminus1 (Jaenicke 2005Elbert et al 2007) Several compounds have been proposed asPBA tracers phospholipids β-13-D-glucan ergosterol manni-tol and arabitol (Womiloju et al 2003 Lau et al 2006 Elbertet al 2007 Bauer et al 2008)

On the other hand volatile organic compounds emittedby the biosphere (BVOCs) may act as precursors of secondaryorganic aerosol (SOA) Isoprene with an estimated globalannual emission of 440ndash660 Tg C yrminus1 accounts for most ofthese emissions (Guenther et al 2006) Small amounts ofalcohols ketones monoterpenes and sesquiterpenes are alsoreleased (Warneck 1988 Alves 2001 Warneke et al 2010)Several studies under laboratory and field conditions haveshown the presence of terpene and isoprene oxidationproducts (Kroll et al 2006 Kleindienst et al 2007) BVOCemissions are estimated to be approximately a factor of 10larger than anthropogenic VOC emissions globally (Seinfeldand Pandis 1998 Atkinson and Arey 2003) It is estimatedthat BVOC oxidation represents the largest SOA global sourceranging from 12 to 70 Tg yrminus1 (Hallquist et al 2009 Finessiet al 2012)

BVOCs are included in different models (eg air qualityforecast global chemistry and climate and regulatoryregional models) due to their important impact on the globaland regional atmospheric chemistry producing secondaryorganic aerosol as well as ozone (Henze and Seinfeld 2006Warneke et al 2010) However modelling BVOCs is not aneasy task since these compounds are emitted by differentplant species which in turn are affected by several factorsGenetic and biochemical factors influence the type of BVOCsemitted by the various species Some studies have focused onthe response of plant emissions to abiotic factors such astemperature light wind or water availability (eg Pentildeuelasand Llusiagrave 2001) Biotic factors such as the interaction withanimals plants or microorganisms have also been studiedand differences have been found as a consequence ofquasi-random events such as herbivore activity in the area(Pentildeuelas and Llusiagrave 2001)

3124 Volcanic eruptions Volcanoes contribute to tropo-spheric and stratospheric pollution by increasing the amountof greenhouse gases sulphur and aerosols affecting theclimate and causing acid rain (Durant et al 2010 andreferences therein) In addition volcanoes are a risk for airtraffic (Prata and Tupper 2009) and health (Horwell andBaxter 2006) and as authors such as Duggen et al (2010)and Langmann et al (2010) have recently pointed outvolcanic ash fallout supplies iron which may enhance oceanproductivity and lead to a drawdown of atmospheric CO2These impacts are limited to important eruptions but duringthese events large numbers of particles are released into theatmosphere at different latitudes altitudes and with differentresidence times (Brimblecombe 1996 Watanabe et al2004) Volcanic emissions are primarily H2O followed byCO2 SO2 HCl and other compounds (eg Bardintzeff andMcBirney 2000) It is extremely difficult to predict emissionsfrom volcanic eruptions because of the wide range of



eruptive styles and their variability (Stohl et al 2011 andreferences therein)

Volcanic eruptions are an important natural source ofprimary and secondary aerosols Among the latter we findsecondary sulphate formed mainly from the oxidation of theSO2 released to the atmosphere in large amounts during theeruptions (Thomas et al 2009) Amounts between 1 and2 Tg of SO2 were injected into the lower stratosphere duringvolcano eruptions such as the one in Kasatochi (Alaska USA2008) or Sarychev (Russia 2009) (Corradini et al 2010Haywood et al 2010) making them the largest volcaniceruptions since Mount Pinatubo (Philippines) and MountHudson (Chile) in 1991 More recently the Eyjafjallajoumlkulleruption (Iceland 2010) seriously distracted aviation inEurope causing important economic losses A number ofstudies have been carried out on emissions from this volcanoeruption and its impacts (Revuelta et al 2012) Variousstudies suggest that between 14 and 36 of the mass ofsecondary sulphate aerosols in the troposphere may be ofvolcanic origin (Chin and Jacob 1996 Graf et al 1997)

Elements such as Al Si S Cl K Ca Ti Mn Fe Cu and Zn arepart of the chemical composition of volcanic eruptions (Allardet al 2000) though in variable concentrations (Miranda et al2004) Themercury emitted by volcanoes has been studied andestimated by several authors (Pirrone et al 2010) andaccording to Mason (2009) on average volcanoes andgeothermal activities release about 90 Mg yrminus1 of mercury tothe atmosphere (~2 of the total contribution from naturalprocesses) Volcanic ashes generally fall within the range of1ndash10 μm although the size interval of the particles released bythe volcanic plumes is very large (Ilyinskaya et al 2010)

If the eruption is strong enough the aerosols may reachthe stratosphere where they have important climaticconsequences worldwide (Vernier et al 2011) Stratosphericvolcanic aerosols have an average lifetime of 1ndash2 years (Gaoet al 2007) However when the injection occurs only intothe troposphere the atmospheric lifetime of troposphericaerosols is about 1 week (Seinfeld and Pandis 2006) Matheret al (2003) have discussed origins and transformations ofvolcanogenic particles in the troposphere covering theirfluxes size distribution composition and morphology andfocusing on sulphur halogen and trace metal compounds

3125 Lightning Lightning is an important source of NOx (NOand NO2) in the atmosphere and as a consequence a source ofsecondary natural nitrate particles (Schumann and Huntrieser2007) In lightning events a peak temperature is reached(28000ndash31000 K) in a lightning channel within the first10ndash20 μs after the return stroke when the air in the channelis totally ionised (MacGorman and Rust 1998 Yu and Turco2001) The next reaction takes place N2+O2rarr2NO The NOproduced can be oxidised into NO2 Cooray et al (2009) haveestimated that the global annual production of NOx is about4 Tg (N) for the total length of channels inside the cloud of atypical ground flash of about 45 km A best estimate value ofabout 5 Tg (N) yrminus1 has been widely accepted for lightning Nproduction

Aerosols and lightning seem to have a bidirectionalinfluence Thus some studies point out a higher lightningflash density near urban areas (Kar et al 2009) Yuan et al(2011) have recently shown that in general lightning activity

is tightly correlated with aerosol loadings at both inter-annualand bi-weekly time scales In this study the authors estimatethat a ~60 increase in aerosol loading leads tomore than 150increase in lightning flashes Aerosols increase lightningactivity through modification of cloud microphysics

32 The chemical composition of aerosols

The following paragraphs briefly describe the main chem-ical compounds forming aerosols

321 Sulphur speciesMost sulphate aerosols in the atmosphere are secondary

sulphates formed by the oxidation of gaseous precursors (withSO2 and dimethyl sulfide ndash DMS ndash as the main contributors)followed by particle formation through nucleation and con-densation processes There are several pathways for sulphateformation such as liquid-phase reactions inside cloud dropletsor oxidation of SO2 with OH via gaseous phase reactions(eg Penner 2001) SO2 is emitted to the atmosphere frombothanthropogenic and natural sources although it has beenestimated that more than 70 of SO2 global emissions arereleased by anthropogenic sources (Whelpdale et al 1996)and fossil fuel combustion is responsible for the vastmajority ofthese emissions Other SO2 sources are biomass burningshipping metal smelting agricultural waste burning pulpand paper processing and a modest volcanic source (Andreaeand Rosenfeld 2008 Smith et al 2011) Anthropogenicsources of SO2 have soared from less than 10 Tg yrminus1 ofsulphur in 1890 to 70ndash75 Tg yrminus1 in 2000 (Dentener et al2006 Ganzeveld et al 2006) According to Smith et al (2011)in their study on anthropogenic sulphur dioxide emissionsfrom 1850 to 2005 SO2 global emissions peaked in the early1970s and decreased until 2000 This can be explained on theone hand by a rapid decrease in the emissions as aconsequence of control mechanisms in developed countriesand on the other hand by a rapid increase registered in theemissions from underdeveloped countries in recent years(Stern 2006 Andreae and Rosenfeld 2008) Smith et al(2011) add the growing importance of international shippingas a factor in the increase of SO2 emissions The main naturalsource of atmospheric sulphur is DMS (Derevianko et al2009) with an annual contribution of 281 (176ndash344) TgS yrminus1 according to Lana et al (2011) Haywood and Boucher(2000) and Andreae and Rosenfeld (2008) have summarisedemission estimations from various sulphur sources

SO2 oxidises to H2SO4 at a speed which is directly linkedto the intensity of solar radiation (Heintzenberg 1985) Thiscompound is not found in the gaseous phase in thetroposphere because of the low sulphuric acid saturationvapour pressure (Meacuteszaacuteros 1999) but it rather condensesrapidly to form droplets of a sulphuric acid solution Undernormal atmospheric conditions these particles are partiallyor totally neutralised by ammonia (NH3) and in the processdepending on relative humidity they may become solids(Wang et al 2008) However the neutralisation of thesulphuric acid generates calcium sulphate (CaSO4) or sodiumsulphate (Na2SO4) in environments with high concentrationsof calcium carbonate (CaCO3) and sodium chloride (NaCl)(Querol et al 1998b Seinfeld and Pandis 2006)



The optical parameters of sulphate aerosols have beenwidely studied (Penner 2001) After greenhouse gases theyconstitute the most important anthropogenic forcing for theclimate Sulphate is essentially an entirely scattering aerosolacross the solar spectrum but with a small degree ofabsorption in the near-infrared spectrum According to IPCC(2007) the radiative forcing thatmay be attributed to sulphateis minus04plusmn02 W mminus2

322 Nitrogen speciesAs in the case of sulphates nitrogen compounds are mainly

of secondary origin and come from the reaction of natural andanthropogenic gaseous precursors These aerosols generallyhave diameters smaller than 25 μm (Putaud et al 2010Squizzato et al 2012) NO3

minus and NH4+ are the main nitrogen

compounds in atmospheric particulate matter The mainprecursor gases emitted by natural and anthropogenic sourcesare NO NO2 N2O and NH3 and nitric acid is the main productgenerated by oxidation in the atmosphere (Meacuteszaacuteros 1999)

The anthropogenic production of secondary nitrate precur-sor gases occurs in the generation of power (gas fuelndashoil andcoal combustion) and in other combustion processes involvinghigh temperatures such as those occurring in the motors ofvehicles and in biomass burning (Pinder et al 2012) On theother hand agricultural activities such as land fertilising are themain source of atmospheric NH3 (McCubbin et al 2002)although it is emitted by other sources including wastecollection vehicles and a number of production processes(Anderson et al 2003 Battye et al 2003)

Natural nitrogen compounds come mainly from soilemissions (nitrification N2O) wildfires (NO2 NO) electricaldischarges (NO) and biogenic emissions (NH3) (Seinfeld andPandis 1998)

The production of secondary nitrate is heavily dependenton the amount of gaseous NH3 and HNO3 and of particulateSO4

2minus as well as on temperature and humidity (Bauer et al2007) Homogeneous (gas-phase reaction of NO2+OH) andheterogeneous (hydrolysis of N2O5 on aerosol surfaces) re-actions are involved in the formation of nitric acid during thedaytime and nighttime respectively (Pathak et al 2009) Innormal conditions the gaseous nitric acid dissolved in liquidmicroparticles reacts with the ammonia in the atmosphereforming particulate ammonium nitrate (EPA 1996)

HNO3ethgTHORN thorn NH3ethgTHORNNH4NO3ethsTHORNAmmoniumnitrate is unstable because of the higher vapour

pressure of NH3 and HNO3 (EPA 1996 Meacuteszaacuteros 1999) so itvolatilises partially at more than 20 degC forming again gaseousnitric acid At more than 25 degC the volatilisation is complete(Schaap et al 2004) This volatilisation may take place in theatmosphere or in the filter where the particulate matter issampled Because of this fact ammonium nitrate possesses amarked seasonality with maximum values in winter andminimum values in summer in areas such as the IberianPeninsula (Querol et al 1998a 1998b 2001) In an acidenvironment (for example acid sulphates non-neutralised byammonium) ammonium nitrate dissociates (Gebhart et al1994) into ammonium sulphate so in acid environments theformation of ammonium nitrate is always conditioned bythe previous neutralisation by ammonium of atmospheric

sulphates (formation of ammonium sulphate) (Pathak et al2009 and references therein) This also explains why ammo-nium sulphate is more stable in the atmosphere and used as atracer for long-range transport (Minguilloacuten 2007)

Nitrate may also be found forming NaNO3 and Ca(NO3)2in acid environments and in environments with highconcentrations of Na+ and Ca2+ (eg as a reaction productwith sea salt or mineral dust) These particles are larger thanammonium nitrate which belongs to the submicron sizefraction (Querol et al 1998b)

Several global model studies (eg Liao and Seinfeld 2005Liao et al 2006) have pointed out that the expected decrease insulphate forcing (SO2 emissions are relatively easy to control)may be counterbalanced in the future by an increase in nitrateaerosols caused by the rapid increase in nitrogen emissionswhich are much more difficult to control Bauer et al (2007)estimate a direct nitrate radiative forcing of minus011 W mminus2and values of minus016 minus01 minus004 minus002 W mminus2 wereregistered by Liao et al (2006) IPCC (2007) Jacobson (2001)and Myhre et al (2006) respectively The lowest nitrateradiative forcings were estimated considering aerosol mixing

323 Carbonaceous speciesCarbonaceous aerosols are a significant fraction of atmo-

spheric aerosols and comprise a wide range of compounds Ithas been estimated that this fraction is between 20 and 50of the PM25 mass in urban and rural locations and up to 70of the PM1 mass (Zhang et al 2007 Querol et al 2009a) Thecarbon in aerosols can be classified into three groups a) thegroup corresponding to carbonates b) elemental carbon (EC)or black carbon (BC) in terms of light absorption andc) organic carbon (OC)

Occasionally with the aim of considering the contributionof other elements such as O N and H the amount ofparticulate organic matter (POM) is estimated from the OCconcentration multiplying it by a factor taking valuesbetween 13 and 22 (Hegg et al 1997 Chazette andLiousse 2001 Turpin and Lim 2001) The factor chosen is afunction of the composition of the aerosol sampled its originand its degree of aging (Stelson and Seinfeld 1981 Puxbaumand Tenze-Kunit 2003)

The carbon found in the form of carbonates (mainly CaCO3

and MgCO3) occurs usually as supermicrometric particlesresuspended from the ground This fraction is neglected inmost studies (Jankowski et al 2008) because of the size andbecause there is no straightforward technique for determiningit (it is usually identified by acidifying the sample anddetermining CO2) However in certain areas andor undercertain atmospheric conditions carbonate aerosol concentra-tions may be significant (Querol et al 2009b) RecentlyKaranasiou et al (2011) have tried to identify and quantifythis fraction by means of thermaloptical analysis protocols

BC the most refractory and polymerised part of theaerosol is generated mainly by fossil-fuel combustion andbiomass burning (Jiang et al 2005 Bond et al 2007) BCparticles have a diameter between 10 nm and 100 nm andthe mass ratio HC is of around 01 (Cachier 1998) BC is onlya minor contributor to aerosol mass but it absorbs radiationin a very effective way (034plusmn025 W mminus2) both in theatmosphere (Koch et al 2007 Quinn et al 2008) and afterdeposition for example on snow (Wang et al 2011b)



eventually playing a role in the melting of glaciers It has beenestimated that BC may be the cause of more than half of theArctic warming observed since 1890 (Shindell and Faluvegi2009) BC has been used as a tracer for exposure to dieselcombustion gases (Fruin et al 2004) and because of itsporosity this compoundmay absorb a wide range of chemicalcomponents for example PAHs (Jiang et al 2005) Thisabsorption capability together with the submicrometric sizeof BC confers this compound a certain degree of toxicity(Knaapen et al 2004) Some studies have tried to relate BCwith cancer but there is no evidence today of a clearcorrelation (CalEPA 2005)

OC the non-absorptive fraction of the carbonaceous aerosol(minus005plusmn005 W mminus2 for fossil fuel OC) may be of eitherprimary or secondary origin Sources of OC are not fully knownespecially the fraction formed by secondary atmosphericprocesses SOA may represent up to 90 of OC even in urbanareas (Gelencseacuter et al 2007) It has been demonstrated that asignificant fraction of OC is formed bywater soluble compounds(WSOC) (Novakov and Penner 1993) so these particlesmay befound in the atmospheric aqueous phase (Sellegri 2002) Thiscomponent is of crucial importance since it may alter theradiative balance of the atmosphere and influence the hydro-logical cycle (Duarte et al 2007) A significant portion of theWSOChas been termed ldquohumic-like substancesrdquo (HULIS) due toits similarity to humic substances from soil and waterHowever it has been recognised that this oligomeric materialmay not be soil-derived based on their predominance in thesubmicrometre PM fraction Thus their origin continuesgathering speculative responses (Baltensperger et al 2005)Evidence of polymerisationoligomerisation formation process-es for SOA from both anthropogenic and biogenic precursorswas lately given (Baltensperger et al 2005)

Combustion processes (road traffic industrial processesetc) are the main sources of primary anthropogenic carbona-ceous particles (OC and EC) (Li et al 2012a) Approximately50 of the secondary anthropogenic carbonaceous particlescome from the evaporation of gasoline and from the gaseousemissions of vehicles (Watson et al 2001) On the other handthe emission of natural organic compounds comesmainly fromthe vegetation the soils and the surface of the oceans andthese emissions produce primary particles (vegetation and soilcompounds such as spores pollen humic and fulvic acidsmicroorganisms and fungi) (Campbell et al 1999 Pan et al2007) as well as secondary particles (resulting from atmo-spheric oxidation of the organic gases released mainly by thevegetation)

Currently no method is available to distinguish betweenprimary and secondary compounds so indirect methods areusually employed to identify them (Castro et al 1999 Pio et al2011) The formation of SOA increases both ambient OC levelsand OCEC ratios OC-to-EC ratios exceeding the expectedprimary emission value are an indication of SOA formation(Cabada et al 2004) However SOA estimates based on theseratios are highly variable depending on sources season andlocation (Khalil and Rasmussen 2003) Using a large set ofmeasurements Pio et al (2011) demonstrated that urbanbackground sites show spatially and temporally consistentminimum OCEC ratios of around 10 for PM10 and 07 forPM25 suggesting that the method could be used as a tool toderive the ratio between OC and EC from fossil fuel combustion

and consequently to differentiate OC from primary andsecondary sources To explore this capability OC and ECmeasurements were performed by the same authors in a busyroadway tunnel in central Lisbon The OCEC ratio whichreflected the composition of vehicle combustion emissionswas in the range of 03ndash04 Additional measurements wereperformed under heavy traffic conditions at two doublekerbside sites located in the centre of Lisbon and Madrid TheOCECminimum ratios observed at both sites were found to bebetween those of the tunnel and those of urban background airsuggesting that minimum values commonly obtained for thisparameter in open urban atmospheres overpredict the directemissions of OC from road transport

In the past few years the term brown carbon has been usedto designate the carbonaceous particles which present opticalfeatures halfway between soot carbon (strongly absorbing)and organic carbon (non-absorbing) Sources of browncarbon are among others humic soils HULIS bioaerosolsand the incomplete combustion of hydrocarbons (Andreaeand Gelencseacuter 2006 Yang et al 2009)

A correct differentiation between OC and EC is anotherimportant challenge The thermalndashoptical measurementtechniques constitute the most employed methods enablingthe differentiation between both constituents thanks to anoptical correction of the pyrolysed organic carbon (charring)which is essential for a less-biased measurement of carbonfractions However large differences in the concentration ofthese two fractions are observed when different methods areused due to the complexity in establishing the point ofseparation between OC and EC (eg Park et al 2005 Cavalliet al 2010) IMPROVE (Interagency Monitoring of PROtectedVisual Environments) NIOSH (National Institute of Occupa-tional Safety and Health) and EUSAAR (European Supersitesfor Atmospheric Aerosol Research) have been the mostwidely thermalndashoptical protocols used in the atmosphericscience community differing in temperature set pointsresidence times at each temperature step and in the use ofreflectance or transmittance for charring correction Cavalli etal (2010) study constitutes one of the most recent workstrying to identify different parameters that can potentiallymagnify the inherent biases affecting the correct separationbetween OC and EC by thermalndashoptical methods

Togetherwith thermalndashoptical andorganic tracer techniquesradiocarbon analysis offers an opportunity to apportion carbo-naceous particulate matter between fossil fuel biomass burningcarbon biological particles and secondary organic aerosol Thecarbon isotope 14C is produced in the upper atmosphere andenters the biological carbon cycle with the relatively constantinitial ratio to 12C (Szidat et al 2006 Ceburnis et al 2011) Onthe other hand 14C is entirely depleted in fossil fuels due toradioactive decay Thus the 14C12C ratio clarifies the contribu-tions of contemporary carbon biomass emissions and fossil fuelemissions In addition the ratio of 13C12C elucidates carbonemissions associated with different plants both terrestrial andoceanic due to preferential photosynthesis uptake routes ofheavier or lighter inorganic carbon isotopes (Huang et al 2010Ceburnis et al 2011) The compounds emitted from C3 plants(minus20permil to minus32permil) have a distinctly different isotope signaturefrom those from C4 plants (minus9permil to minus17permil) (Ma et al 2010)Therefore the combination of ratios of 12C 13C and 14C allowsthe quantification of different carbon source contributions to



carbonaceous samples The variations in the isotopic composi-tion of aerosols can be attributed to anthropogenic inputsor biomass burning Anthropogenic activities usually releaseslight 13C-enriched compounds and biomass burning producematerials with the same carbon isotopic composition as bio-mass burnt Additional variation of the isotopic composition ofcompounds is due to photochemical oxidation Themore readilyandmore complete reactionmakes a residual part of compoundsheavier in the carbon isotope composition (Ma et al 2010 andreferences therein)

Stable carbon isotope analyses of atmospheric particleshave been widely used for source identification purposes(eg Cao et al 2011 2012) For instance Widory et al (2004)used a combination of carbon and lead isotopes to differentiatebetween aerosol sources such as road traffic versus industrialemissions in Paris Agnihotri et al (2011) used data for carbonand nitrogen isotopes in aerosols to identify potential aerosolsources for India and the Northern Indian Ocean Stable carbonisotope ratios have been determined for the OC and ECfractions of particles from Chinese cities and it has beenshown that these ratios are potentially useful for identifyingthe sources for carbonaceous pollutants (Huang et al 2010Maet al 2010 Cao et al 2011 2012) Stable carbon isotopeanalysis has also been attempted to apportion marine aerosolorganic matter on several occasions (eg Miyazaki et al 2010)A number of studies have even endeavoured compoundspecific stable carbon analysis as a technique for sourceidentification For example Kim et al (2005) and Zhang et al(2009a) developed an isotope analysis of PAHs Turekian et al(2003)were able to derive isotope ratio of oxalate attributing itto mostly marine precursors Li et al (2010) developed amethod for isoprene biomarkers Fisseha et al (2006) Wangand Kawamura (2006) and Ma et al (2010) carried out stablecarbon analysis of organic acids

4 Suggestions for further research

The wide range of aerosol sources and sinks the complexand highly variable chemical composition of particulatematterthe size distributions the complexity of formation processesand processing the multiple impacts and the importantspatialndashtemporal variation are all evidence of the need tocontinue studying atmospheric particulate matter in depth

Much progress has been made since the beginning ofaerosol science but there are still many aspects that requirefurther investigation In order to elucidate some of the mainopen questions associated with aerosol sources chemicalcomposition and their effects on atmospheric processes andclimate are synthesised in this section Taking into account thatthe organic aerosol (OA) components account for a largesometimes even dominant fraction of the atmospheric partic-ulate matter the discussion is mainly focused on this aerosoltype

Fig 1 portrays the complementary nature of the mostimportant techniques used for the analysis of the organiccontent of aerosols Techniques enabling organic speciationsuch as gas chromatographyndashmass spectrometry (GCndashMS) orliquid chromatographyndashmass spectrometry (LCndashMS) canonly contribute to the resolution of a small mass fraction ofthe organic aerosol On the other hand thermalndashoptical OCECanalysers can quantify 100 of the OCmass in a relatively short

time but do not provide any speciation details Complemen-tary techniques such as aerosol mass spectrometer (AMS)Fourier transform infrared spectroscopy (FTIR) and nuclearmagnetic resonance (NMR) are able to analyse most of theorganic aerosol mass supplying resolution of some functionalgroups or organic classes The perfect instrument combiningselectivity and complete mass resolution still does not existBecause of the particularly complex chemical composition andthe degree to which OA can be altered chemically andphysically in the atmosphere it is dubious that we will everbe able to entirely characterise all organic species throughouttheir lifetime (Fuzzi et al 2006) Improvements of measure-ments techniques are required including (i) development andapplication of powerful and efficient instrumentation for theidentification and quantification of SOA constituents in bothlaboratory and field experiments (eg online and single particleaerosol mass spectrometry isotope analysis) (ii) developmentand optimisation of physical and chemical measurementtechniques for nanometre-sized particles clusters and ions(eg ion spectrometer single particle MS) (iii) further advance-ment on artefact-free aerosol sampling for organic compoundsand a standardised separation protocol for measuring OCECand (iv) development of instrumentation andor analyticaltechniques to understanding of organic composition at thefunctional group or structural level in a more complete wayin terms of bulk- size-segregated and individual aerosolparticles Despite improvements in measurement devicesand analytical techniques the fraction of constituentsparticularly organic compounds that cannot be identifiedis still high Therefore analytical methodsmust receivemoreattention to provide a complete mass balance (Jacobson etal 2000)

There is emerging evidence from both smog-chamber andambient aerosol experiments that aromatic volatile organiccompounds isoprene and monoterpene oxidation productsoligomerise readily in the particle phase under both acidic andnonacidic conditions forming constituents like organosulphatesand organonitrates (Claeys et al 2004 Reemtsma et al 2006Dron et al 2008 Lukaacutecs et al 2009) which may explain a largepart of the till now unidentified fraction of SOA However all ofthese studies made so far have lacked the quantitative aspecthow important this class of compounds can be on a mass basisThis is because techniques used are not appropriate to resolveorganic sulphur or nitrogen levels in bulk Thus it is very tricky tointegrate updated information into atmospheric models and theextent of effects these compounds possibly play in thetroposphere remains unknown Although recent studies havepointed out the relationship between SOA and human healthimpacts (Baltensperger et al 2008 De Bruijne et al 2009) andclimate (Hallquist et al 2009 ODonnell et al 2011) this subjectis in its early stages and needs further research A completeunderstanding of SOA optical properties composition (eg waterinsoluble organic matter HULIS oligomers etc) formation orquantification still needs solid research under field and labora-tory conditions linked to modelling studies and technologydevelopment (Kroll and Seinfeld 2008 Hallquist et al 2009)More environmental chamber and laboratory experimentsunder atmospherically relevant and realistic conditions aredesirable to clarify SOA formation pathways in particularheterogeneous and multiphase reactions as well as organicaerosol aging processes These studies will help to understand



the reactional mechanisms and kinetics of the physical andchemical processes and should be combined with chemicalmodelling studies at different scales (Fuzzi et al 2006) Furtherlaboratory studies are required to make clear the mechanismsand kinetics of nucleation and growth of newparticles aswell toassemble thermodynamic data of SOA components as a functionof distinct parameters such as temperature composition surfacetensions densities vapour pressures activities etc Anotherrecommended research direction focuses on chamber studiesinvolving several organic precursors of biogenic and anthropo-genic origins leading to small and highly oxygenated species orlarge polymers (HULIS) through heterogeneous reaction Addi-tionally under controlled conditions the role of OA as ice nucleior CCN under typical conditions of the upper troposphere shouldbe addressed Also there is still room for laboratory studies ofaerosol water uptake (ie hygroscopicity and activation) for OAand OAmixed with inorganic species and soot These laboratorystudies should be complemented and validated with fieldmeasurements under real atmospheric conditions

In fact progress on resolving open questions requires notonly laboratory but also field experiments Thus field mea-surements on aerosol water uptake (ie hygroscopicity andactivation) and new particle formation with comprehensivephysical and chemical analyses of particles clusters and ionscombined with detailed meteorological data should betargeted To test and validate laboratory chamber and modelresults it is necessary to combine Lagrangian observational

approaches with air parcel and process models (Lohmann andLeck 2005) In order to perform studies of the importance ofdifferent sources and sink processes affecting the aerosol it isdesirable tomake use of simultaneousmeasurements of aerosolproperties on a regional scale This type of measurementapproach gives a relevant connection both in space and timeoften lacking in previous investigations (Tunved et al 2004)Recent research at some stations has mainly focused on thelocal properties of the aerosol and sourcendashreceptor relation-ships Particularly well studied is the role of nucleation on newparticle formation in the boreal environment (eg Nilsson et al2001a 2001b Kulmala et al 2004 2011) However studies ofhow the properties of aerosol components evolve fromemission at the source to locations downwind both beforeand after cloud-processing are still lacking for many areas Anoverarching goal is to understand the chemical transformationand removal processes of aerosols oxidants and their pre-cursors during the intercontinental transport process To makethis understanding possible measurements from a Lagrangianplatform would be ideal ie a platform that moves with anair mass during the total transport process Such an ideal isnot possible due to the limited range and endurance ofexisting aircraft A practical approximation to this ideal is apseudo-Lagrangian study where one or more aircraft makemultiple sequential sampling flights into the same air massduring the time required for the intercontinental transport ofthe air mass

Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0

Perfect instrumentAMS

PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS

Fig 1 Techniques currently devoted to the organic aerosol analysis AMSmdash aerosol mass spectrometer CImdash chemical ionisation EAmdash electron attachment OCECmdash

organic and elemental carbon FTIRmdash Fourier transform infrared spectroscopy GCndashMSmdash gas chromatographyndashmass spectrometry LCndashMSmdash liquid chromatographyndashmass spectrometry 2D-GCndashMS mdash two dimensional gas chromatographyndashmass spectrometry HR-ToF-AMS mdash high resolution time-of-flight massspectrometer NMR mdash nuclear magnetic resonance PBTDMSS mdash particle beam thermal desorption mass spectrometer PILS-OC mdash particle into liquid sampler fororganic carbon VUV mdash vacuum ultra-violetAdapted from Hallquist et al (2009)



The identification characterisation and control of thesources emitting aerosols containing toxic material are ofspecial relevance so that regulations in that area may beimproved tominimise these emissions It is therefore necessaryto keep in mind that future regulations should focus not onlyon aerosol mass load and size but also on the specific com-ponents in order to reduce or minimise adverse health effectsand improve medical treatments (Poumlschl 2005 Mijic et al2010) These regulations should not forget the important roleof cross-border atmospheric pollution something which willrequire cooperation between countries Enhancing this type ofinternational studies will make it possible to design and carryout air quality control systems and short-term actions Thereare several countries which still lack air quality regulationsmainly developing countries but contribute important loads ofparticles and pollutants to the atmosphere The currentregulations for controlling emissions have considerably re-duced exhaust emissions However non-exhaust emissionsfrom road vehicles are unabated Improved information on thechemical composition of these emissions is important toimplement source-oriented mitigation measures health-related studies and to model source contributions The intro-duction of biofuels hydrogen fuel cells and electric poweredvehicles represents an important promise for the near futureThe direct emissions from these processes are less importantthan those from fossil fuels but we need to study and quantifythe indirect emissions linked to the production of these fuelssince they may be an important source of particles or theirprecursors (Skeie et al 2009) All the processes involved in therelease into the atmosphere of particles and their precursorsfrom the industrial sector must be typified and attempts mustbe made to minimise these emissions Fugitive emissions needto be characterised and more accurately quantified In spite ofbeing a major source of OA in many regions emissions fromcooking have not yet been extensively characterised Theseemissions depend strongly on the cooking method and foodingredients and nothing is known about the speciation ofparticle emissions according to the typical gastronomy inmanyregions Also much research must still be done to correctlyestimate totals of garbage burnt worldwide particle emissionrates and their features (chemical composition optical charac-teristics size distribution etc) Furthermore characterisingand quantifying emissions frombiomass burning are importantsteps in establishing emission profiles of wood species growingworldwide in order to improve emission inventories andcontribute to source apportionment Aspects related to thechemical composition the aging of aerosols after emission andtheir impacts on radiative forcing are crucial points whichrequire further investigation

Emissions from natural sources are less well quantifiedmainly because of the difficulties of measuring emission ratesin the field and the unpredictable nature of the events Oftenemissions must be inferred from ambient observations atsome distance from the actual source The natural emissionsin general can vary noticeably over space and time

Concerning natural sources one of the most importantchallenges focuses on distinguishing anthropogenic and naturalfractions of mineral dust particles (Forster et al 2007) Someauthors have speculated about the possibility of estimatinganthropogenic dust particles on the basis of aerosols emitted byhuman-disturbed soils In other words agricultural activities

may cause an increase in the aerosol organic matter fractionandmaymodify its size distribution However no evidence hasbeen registered until now (Formenti et al 2011) Besides thenatural mineral aerosol from arid regions dust emissions fromhuman activities such as from farming practices and land-usechanges likewise need to be quantified Improved estimates ofdirect radiative forcing by dust will require improved charac-terisation of the spatial variability in particle characteristics toafford reliable information on dust optical properties Thisincludes constraints on (Durant et al 2010 Formenti et al2011 Redmond et al 2010) (i) particle-size distributionincluding discrimination of particle subpopulations and quan-tification of the amount of dust in the sub-10 μm tob01 μmmass fraction (ii) particle composition specifically the abun-dance of iron oxides and whether particles consist of single ormulti-mineral grains (iii) particle shape including degree ofsphericity and surface roughness as a function of size andmineralogy and (iv) the degree to which dust particles areaggregated together The use of techniques that measure thesize composition and shape of individual particles will providea better basis for optical modelling

In recent years the impact of PBA on atmospheric processeshas been investigated with increasing interest and a wealth ofnew information and insights has been gained (eg Bauer et al2008 Bowers et al 2009 2011 Burrows et al 2009a 2009bHeald and Spracklen 2009 Iinuma et al 2009) Severalresearch activities should be pursued in future studies of PBA(Despreacutes et al 2012) (i) develop efficient and consistentanalytical techniques for their identification and quantification(ii) apply advanced and standardised techniques to determinethe abundance anddiversity of PBA and their seasonal variationat regional and global scales (atmospheric biogeography)(iii) determine their emission rates optical properties icenuclei and CCN activity in field measurements and laboratoryexperiments and (iv) use field and laboratory data to constrainnumerical models of atmospheric transport transformationand climate effects of PBA

As measurements are limited spatially and temporally therole of the ocean as a source of aerosols and their potential tointerfere with the climate remain unclear Moreover despitesome studies on the occurrence of chemical compounds inmarine aerosols (Wang et al 2006 Alves et al 2007a) a broaddepiction on the nature of their organic matter remainsunavailable Despite scattered research in various oceanograph-ic fields a general understanding of the role of the SML incontaminant concentration and pollutant transport via marineaerosol is not yet available Early work suggests intercontinen-tal transport of viable pathogenic microbes which may beenriched up to 3 orders of magnitude in marine aerosolsrelative to SML (Aller et al 2005) Knowledge of the effect ofsurfactants on aerosol production by bubble bursting and therole of these surface-active agents for biogeochemical fraction-ation and pollutant transport via marine aerosols are in theearly stages (Sellegri et al 2006)

Volcanic eruptions are an important natural cause ofclimate change on many timescales To detect and apportionanthropogenic impacts on climate including effects ofgreenhouse gases aerosols and ozone-depleting chemicalsit is essential to quantify the natural fluctuations so as toseparate them from anthropogenic fluctuations in the climaterecord (Robock 2000) Many aspects related to volcanic



emissions need a much more in deep investigation Amongothers these include gas-to-particle conversion and removalmechanisms radiative properties and climatic effects ofstratospheric aerosols improved satellite and in situ mea-surements (global observations of stratospheric aerosoloptical properties and Lidar measurements of aerosols) insitu measurements of tropospheric aerosol optical propertieshealth hazards of tropospheric volcanic gases and aerosolsetc It is important to obtain accurate measurements ofvolcanic aerosols not only because of their importance forclimate but also to allow a higher degree of accuracy inremote sensing of surface properties such as sea surfacetemperature ocean colour and land surface propertiesDuring major volcanic eruptions satellite monitoring ofstratospheric chemical and physical properties is alsosignificantly affected by aerosols The fertilising potential ofvolcanoes in the marine environment is poorly understoodSatellite images and drill core data from scientific oceandrilling illustrate that huge amounts of volcanic ash havebeen deposited in the marine environment Neverthelessrelatively little still is known about the role of volcanoes forthe surface ocean nutrient budget and how volcanic activitymay affect marine primary productivity carbon cycles andclimate in the Earths history (Duggen et al 2010) Oceanicfertilisation with volcanic ash is a process that has largelybeen unnoticed in marine sciences and that its significancefor the marine biogeochemical iron-cycle might have beenunderestimated so far (Duggen et al 2010 Stohl et al2011) Furthermore improvements in the quantification ofHBr emissions constitute an important challenge as they areconsidered a key factor in ozone depletion by volcanoes(Roberts et al 2009) Based on satellite observations it hasbeen recently established that lightning activity is tightlycorrelated with aerosol loadings through modification ofcloud microphysics in particular in areas affected by volcanicplumes (Yuan et al 2011) The possible aerosol effects onlightning activity and structure of hurricanes have also beenshown (Khain et al 2008) However more detailed in-vestigations of the bidirectional lightningndashaerosol interac-tions are required (Wang et al 2011c)

Regarding source apportionment several models havebeen developed in order to identify the contribution ofdifferent sources such as chemical mass balance (CMB)principal component analysis (PCA) or positive matrixfactorization (PMF) (Viana et al 2008) Currently specialattention has been focused on PMF receptor model In thecase of Europe PMF has been widely used for understandingsource impacts on European PM levels (Amato et al 2009Richard et al 2011) However concerning the application ofPMF the major weakness in Europe or other regions incomparison to North America is the scarcity of suitable highquality ambient datasets in which multiple components ofPM have been measured over a long period On the otherhand most of the source profiles used in CMB receptormodelling have been obtained for USA activities refer almostexclusively to primary PM25 and do not encompass someimportant sources For example most traffic emission pro-files have indeed been obtained in US studies However theEuropean fleet (or those from other regions) is quite differentfrom the US fleet with lower engine power and a muchhigher percentage of diesel vehicles in the old continent

(Plotkin 2007) Thus when using SPECIATE (EPAs repositoryof PM speciation profiles of air pollution sources) or othersource profile databases obtained for the US as inputs toCMB receptor models or to verify profiles derived fromambient measurements using multivariate receptor mod-els (eg PMF) a lack of accuracy of emission estimatesfor specific source categories is likely to occur Thus it isdesirable to obtain site-specific source profiles

The ratios of the carbon isotopes 13C and 14C to the mostcommon carbon isotope 12C have been used with somesuccess to demonstrate the sources of carbonaceous aerosolsThese methods remain some of the most powerful toolsavailable for source determination (eg Szidat et al 2006Ceburnis et al 2011 Gilardoni et al 2011) Although somesources have already been characterised isotopically thisresearch should be extended It is recommended that thesemeasurements are done on a more regular basis with con-current chemical measurements of ambient aerosol

Climate change and population development in the 21thcentury are expected to cause increases in atmosphericaerosol concentrations There is a clear need for enhancedknowledge of interactions between changing atmosphericaerosols and the Earth Systems to increase confidence in ourunderstanding of how and why the climate and environmenthave changed and to develop improved predictive capabili-ties for integrated assessments of climate change in thefuture In fact the uncertainty in evaluating aerosol impactson climate must be much reduced from its present level topermit significant predictions of future climate At presentthis uncertainty is dominated by the aerosol component(Loeb and Su 2010 Peacutereacute et al 2011) Moreover assessmentof effects on climate must consider high spatial and temporalvariations of aerosol amounts and properties as well as itsinteractions with clouds and precipitation Thus the wayforward needs more confident estimates of aerosol radiativeforcing which in turn requires better observations improvedmodels and a synergistic approach To fulfil this demandinggoal it will be necessary to sustain current and expandsatellite capabilities andor surface observation networksObservation should be enlarged with routine measurementsof other key parameters including aerosol composition andsize distribution cloud microphysical properties and precip-itation variables with state-of-art techniques to study theatmospheric processes to expand the database of detailedaerosol chemical physical and opticalradiative characteris-tics to validate remote-sensing retrieval products and toevaluate chemistry transport models The best approach is tomake synergistic employment of measurements from multi-ple platforms sensors and instruments presenting comple-mentary capabilities The deployment of these instrumentsacross the globe on ships at ground-based sites and onaircrafts has greatly expanded over the past two decadesHowever further advances are needed to make this newlydeveloped instrumentation more affordable and turn-key sothat it can be deployed more widely to characterise aerosolproperties at a variety of sites worldwide Progress in betterquantifying aerosol impacts on climate will need betterrepresentation of aerosol composition and absorption in theglobal models better theoretical understanding of small scaleprocesses influencing the aerosolndashcloud interactions andlifetime improved parameterisations of cloud and aerosol



microphysics improved understanding of aerosol effects onsurface radiation and hydrological cycles better knowledge ofthe regional and seasonal diversities of aerosols long-termdata record having consistent accuracy and high qualitysuitable for detecting changes in aerosol amount and typeover decadal time scales more refined climate model simula-tions with coupled aerosol and cloud processes improvedsatellite observations of aerosol type aerosol single-scatteringalbedo vertical distributions and aerosol radiative effect at thetop of the atmosphere and more coordinated field measure-ments to supply constraints on aerosol chemical physical andoptical properties

5 Concluding remarks

Aerosol science is a complex discipline requiring deepinvestigation for a comprehensive understanding Severalprocesses and interactions are involved in atmospheric aero-sols many of which are difficult to identify andor quantifySources and sinks morphology chemical composition sizeinteractions impacts etc make it difficult to completelycharacterise aerosols For this reason it becomes necessary tocontinue studying different aspects of atmospheric aerosols inan integrated and multidisciplinary way The broad range ofproperties associated with atmospheric aerosols requires thatan integrated approach be used for their meaningful investiga-tion The combination of field studies laboratory experimentsand modelling is crucial for refining source apportionmentestimates accurately quantifying the spatial and temporaldistributions of the tropospheric aerosol burdens improvingemission inventories and narrowing the gap between thecurrent understanding of the contribution of both anthropo-genic and natural aerosols to radiative forcing By discussingsome important features related to the aerosol science in thismanuscript it is expected to encourage and strengthen thecooperation between research groups aiming at benefittingfrom synergies and complementarities

Acknowledgments

Ana I Calvo and Ana M Vicente acknowledge the posdocand PhD grants SFRHBPD648102009 and SFRHBD485352008 respectively from the Portuguese Science Foundation(FCT) This study was partially supported by the RegionalGovernment of Castile and Leoacuten (grant LE039A10-2) and bythe Spanish Ministry of Education (grant TEC2010-19241-C02-01) Part of the bibliographical compilation was donewithin the project ldquoSource apportionment of urban emissionsof primary particulate matterrdquo (URBE) PTDCAAC-AMB1179562010 funded by FCT

Appendix A Supplementary data

Supplementary data to this article can be found online athttpdxdoiorg101016jatmosres201209021

References

Agnihotri R Mandal TK Karapurkar SG Naja M Gadi R AhammmedYN Kumar A Saud T Saxena M 2011 Stable carbon and nitrogen

isotopic composition of bulk aerosols over India and northern IndianOcean Atmos Environ 45 2828ndash2835

Agricola G 1912 De re metallica Reprint by Dover Press of the 1912Edition of the Translation by Herbert and Lou Henry Hoover

Agus EL Lingard JJN Tomlin AS 2008 Suppression of nucleation modeparticles by biomass burning in an urban environment a case studyJ Environ Monit 10 979ndash988

Ahn YC Lee JK 2006 Physical chemical and electrical analysis of aerosolparticles generated from industrial plants J Aerosol Sci 37 187ndash202

Aitken J 1890 On improvements in the apparatus for counting the dustparticles in the atmosphere Proc R Soc Edinb 16 135ndash172

Akagi SK Yokelson RJ Wiedinmyer C Alvarado MJ Reid JS Karl TCrounse JDWennberg PO 2011 Emission factors for open and domesticbiomass burning for use in atmospheric models Atmos Chem Phys 114039ndash4072

Allard P Aiuppa A Loyer H Carrot F Gaudry A Pinte G Michel ADongarragrave G 2000 Acid gas and metal emission rates during long-livedbasalt degassing at Stromboli Volcano Geophys Res Lett 27 1207ndash1210

Aller JY Kuznetsova MR Jahns CJ Kemp PF 2005 The sea surfacemicrolayer as a source of viral and bacterial enrichment in marineaerosols J Aerosol Sci 36 801ndash812

Alonso-Blanco E Calvo AI Fraile R Castro A 2012 The influence ofwildfires on aerosol size distributions in rural areas SciWorld J 12 httpdxdoiorg1011002012735697

Alves CA 2001 Origem e composiccedilatildeo da mateacuteria orgacircnica presente nosaerossoacuteis atmosfeacutericos PhD Thesis University of Aveiro

Alves C Oliveira T Pio C Silvestre AJD Fialho P Barata F Legrand M2007a Characterisation of carbonaceous aerosols from the AzoreanIsland of Terceira Atmos Environ 41 1359ndash1373

Alves C Pio C Campos E Barbedo P 2007b Size distribution ofatmospheric particulate ionic species at a coastal site in PortugalQuim Nova 30 1938

Alves CA Gonccedilalves C EvtyuginaM Pio CAMirante F PuxbaumH 2010Particulate organic compounds emitted from experimental wildland firesin a Mediterranean ecosystem Atmos Environ 44 2750ndash2759

Alves C Vicente A Monteiro C Gonccedilalves C Evtyugina M Pio C 2011aEmission of trace gases and organic components in smoke particles from awildfire in a mixed-evergreen forest in Portugal Sci Total Environ 4091466ndash1475

Alves C Vicente A Nunes T Gonccedilalves C Fernandes AP Mirante FTarelho L Saacutenchez De La Campa AM Querol X Caseiro A Monteiro CEvtyugina M Pio C 2011b Summer 2009 wildfires in Portugal emissionof trace gases and aerosol composition Atmos Environ 45 641ndash649

Amato F Pandolfi M Escrig A Querol X Alastuey A Pey J Perez N HopkePK 2009 Quantifying road dust resuspension in urban environment bymultilinear engine a comparisonwith PMF2 Atmos Environ 43 2770ndash2780

Anderson N Strader R Davidson C 2003 Airborne reduced nitrogen ammoniaemissions from agriculture and other sources Environ Int 29 277ndash286

Andreae MO Gelencseacuter A 2006 Black carbon or brown carbon Thenature of light-absorbing carbonaceous aerosols Atmos Chem Phys 63131ndash3148

Andreae MO Merlet P 2001 Emission of trace gases and aerosols frombiomass burning Global Biogeochem Cycles 15 955ndash966

Andreae MO Rosenfeld D 2008 Aerosolndashcloudndashprecipitation interac-tions Part 1 The nature and sources of cloud-active aerosols Earth SciRev 89 13ndash41

Atkinson R Arey J 2003 Gas-phase tropospheric chemistry of biogenic volatileorganic compounds a review Atmos Environ 37 (Suppl 2) 197ndash219

Avy AP 1956 Les Aeacuterosols Dunod (292 pp)Badarinath KVS Latha KM Chand TRK Gupta PK 2009 Impact of

biomass burning on aerosol properties over tropical wet evergreenforests of Arunachal Pradesh India Atmos Res 91 87ndash93

Balkanski Y Schulz M Claquin T Guibert S 2007 Reevaluation ofmineral aerosol radiative forcings suggests a better agreement withsatellite and AERONET data Atmos Chem Phys 7 81ndash95

Baltensperger U Kalberer M Dommen J Paulsen D Alfarra MR Coe HFisseha R Gascho A Gysel M Nyeki S Sax M Steinbacher MPrevot ASH Sjogren S Weingartner E Zenobi R 2005 Secondaryorganic aerosols from anthropogenic and biogenic precursors FaradayDiscuss 130

Baltensperger U Dommen J Alfarra MR Duplissy J Gaeggeler KMetzger A Facchini MC Decesari S Finessi E Reinnig C 2008Combined determination of the chemical composition and of healtheffects of secondary organic aerosols the POLYSOA Project J AerosolMed Pulm Drug Deliv 21 145ndash154

Bardintzeff JM McBirney AR 2000 Volcanology Jones amp BartlettPublishers Paris

Barman S Singh R Negi M Bhargava S 2008 Ambient air quality ofLucknow City (India) during use of fireworks on Diwali Festival EnvironMonit Assess 137 495ndash504



Barrett SRH Britter RE Waitz IA 2010 Global mortality attributable toaircraft cruise emissions Environ Sci Technol 44 7736ndash7742

Battye W Aneja VP Roelle PA 2003 Evaluation and improvement ofammonia emissions inventories Atmos Environ 37 3873ndash3883

Bauer SE Koch D Unger N Metzger SM Shindell DT Streets DG2007 Nitrate aerosols today and in 2030 a global simulation includingaerosols and tropospheric ozone Atmos Chem Phys 7 5043ndash5059

Bauer H Claeys M Vermeylen R Schueller E Weinke G Berger APuxbaum H 2008 Arabitol and mannitol as tracers for the quantifica-tion of airborne fungal spores Atmos Environ 42 588ndash593

Beddows DCS Harrison RM 2008 Comparison of average particlenumber emission factors for heavy and light duty vehicles derivedfrom rolling chassis dynamometer and field studies Atmos Environ 427954ndash7966

Besombes J-L Maitre A Patissier O Marchand N Chevron N StoklovM Masclet P 2001 Particulate PAHs observed in the surrounding of amunicipal incinerator Atmos Environ 35 6093ndash6104

Bond TC Streets DG Yarber KF Nelson SM Woo J-H Klimont Z2004 A technology-based global inventory of black and organic carbonemissions from combustion J Geophys Res 109 D14203

Bond TC Bhardwaj E Dong R Jogani R Jung S Roden C Streets DGTrautmann NM 2007 Historical emissions of black and organiccarbon aerosol from energy-related combustion 1850ndash2000 GlobalBiogeochem Cycles 21 (GB2018)

Bowers RM Lauber CL Wiedinmyer C Hamady M Hallar AG Fall RKnight R Fierer N 2009 Characterization of airborne microbialcommunities at a high-elevation site and their potential to act asatmospheric ice nuclei Appl Environ Microbiol 75 5121ndash5130

Bowers RM Mcletchie S Knight R Fierer N 2011 Spatial variability inairborne bacterial communities across land-use types and theirrelationship to the bacterial communities of potential source environ-ments ISME J 5 601ndash612

Brimblecombe P 1996 Air Composition and Chemistry CambridgeUniversity Press

Brimblecombe PE 1998 In Fenger J Hertel O Palmgren F (Eds) UrbanAir Pollution European Aspects Kluwer Academic Publishers TheNetherlands pp 7ndash21

Brown WK Wohletz KH 1995 Derivation of the Weibull distributionbased on physical principles and its connection to the RosinndashRammlerand lognormal distributions J Appl Phys 78 2758ndash2763

Bukowiecki N Lienemann P Hill M Furger M Richard A Amato FPreacutevocirct A Baltensperger U Buchmann B Gehrig R 2010 PM10

emission factors for non-exhaust particles generated by road traffic in anurban street canyon and along a freeway in Switzerland Atmos Environ44 2330ndash2340

Buonanno G Morawska L Stabile L 2009 Particle emission factors duringcooking activities Atmos Environ 43 3235ndash3242

Burrows SM Butler T Joumlckel P Tost H Kerkweg A Poumlschl U LawrenceMG 2009a Bacteria in the global atmosphere mdash part 2 modeling ofemissions and transport between different ecosystems Atmos ChemPhys 9 9281ndash9297

Burrows SM Elbert W Lawrence MG Poumlschl U 2009b Bacteria in theglobal atmosphere mdash part 1 review and synthesis of literature data fordifferent ecosystems Atmos Chem Phys 9 9263ndash9280

Cabada JC Pandis SN Subramanian R Robinson AL Polidori A Turpin B2004 Estimating the secondary organic aerosol contribution to PM25 usingthe EC tracer method Aerosol Sci Technol 38 140ndash155

Cachier H 1998 Carbonaceous combustion aerosols In Harrison RM VanGrieken R (Eds) Atmospheric Particles Wiley New York pp 295ndash348

Cadle SH Ayala A Black KN Graze RR Koupal J Minassian F MurrayHB Natarajan M Tennant CJ Lawson DR 2008 Real-world vehicleemissions a summary of the Seventeenth Coordinating Research CouncilOn-Road Vehicle Emissions Workshop J Air Waste Manage 58 3

Cakmur RV Miller RL Perlwitz J Geogdzhayev IV Ginoux P Koch DKohfeld KE Tegen I Zender CS 2006 Constraining the magnitude ofthe global dust cycle by minimizing the difference between a model andobservations J Geophys Res 111 D06207

CalEPA 2005 Chemicals Known to the State to Cause Cancer orReproductive Toxicity California Environmental Protection AgencyOffice of Environmental Health Hazard Assessment (OEHHA)

Calvo AI Olmo FJ Lyamani H Alados-Arboledas L Castro A Fraile RFernaacutendez-Raga M 2010a Winter precipitation chemistry in thebackground EMEP station in Viacuteznar (Granada Spain) (2002ndash2006)Atmos Res 96 408ndash420

Calvo AI Pont V Castro A Mallet M Palencia C Roger JC DubuissonP Fraile R 2010b Radiative forcing of haze during a forest fire in SpainJ Geophys Res 115 D08206

Calvo AI Castro A Pont V Cuetos M Saacutenchez ME Fraile R 2011Aerosol size distribution and gaseous products from the oven-controlledcombustion of straw materials Aerosol Air Qual Res 11 616ndash629

Campbell ID Mcdonald K Flannigan MD Kringayark J 1999 Long-distance transport of pollen into the Arctic Nature 399 29ndash30

Cao JJ Chow JC Tao J Lee SC Watson JG Ho KF Wang GH ZhuCS Han YM 2011 Stable carbon isotopes in aerosols from Chinesecities influence of fossil fuels Atmos Environ 45 1359ndash1363

Cao JJ Zhu CS Tie XX Geng FH Xu HM Ho SSH Wang GH HanYM Ho KF 2012 Characteristics and sources of carbonaceous aerosolsfrom Shanghai China Atmos Chem Phys Discuss 12 16811ndash16849

Carslaw KS Boucher O Spracklen DV Mann GW Rae JGLWoodward S Kulmala M 2010 A review of natural aerosol in-teractions and feedbacks within the Earth system Atmos Chem Phys10 1701ndash1737

Castro LM Pio CA Harrison RM Smith DJT 1999 Carbonaceous aerosolin urban and rural European atmospheres estimation of secondaryorganic carbon concentrations Atmos Environ 33 2771ndash2781

Castro A Alonso-Blanco E Gonzaacutelez-Colino M Calvo AI Fernaacutendez-Raga M Fraile R 2010 Aerosol size distribution in precipitation eventsin Leoacuten Spain Atmos Res 96 421ndash435

Cavalli F Viana M Yttri KE Genberg J Putaud JP 2010 Toward astandardised thermalndashoptical protocol for measuring atmosphericorganic and elemental carbon the EUSAAR protocol Atmos MeasTech 3 79ndash89

Ceburnis D Garbaras A Szidat S Rinaldi M Fahrni S Perron N WackerL Leinert S Remeikis V Facchini MC Prevot ASH Jennings SGRamonet MCD ODowd 2011 Quantification of the carbonaceousmatter origin in submicron marine aerosol by 13C and 14C isotopeanalysis Atmos Chem Phys 11 8593ndash8606

Chahine T Schultz B Zartarian V Subramanian SV Spengler J HammittJ Levy JI 2011 Modeling geographic and demographic variability inresidential concentrations of environmental tobacco smoke using nationaldata sets J Exposure Sci Environ Epidemiol 21 646ndash655

Chazette P Liousse C 2001 A case study of optical and chemical groundapportionment for urban aerosols in Thessaloniki Atmos Environ 352497ndash2506

Chen Y Zhi G Feng Y Liu D Zhang G Li J Sheng G Fu J 2009Measurements of black and organic carbon emission factors forhousehold coal combustion in China implication for emission reductionEnviron Sci Technol 43 9495ndash9500

Cherrie JW Aitken RJ 1999 Measurement of human exposure tobiologically relevant fractions of inhaled aerosols Occup Environ Med56 747ndash752

Chien S Huang YJ Chuang SC Yang HH 2009 Effects of biodieselblending on particulate and polycyclic aromatic hydrocarbon emissionsin nanoultrafinefinecoarse ranges from diesel engine Aerosol AirQual Res 9 18ndash31

Chin M Jacob DJ 1996 Anthropogenic and natural contributions totropospheric sulfate a global model analysis J Geophys Res 10118691ndash18699

Chirico R Decarlo PF Heringa MF Tritscher T Richter R Prevot ASHDommen J Weingartner E Wehrle G Gysel M Laborde MBaltensperger U 2010 Impact of after treatment devices on primaryemissions and secondary organic aerosol formation potential from in-use diesel vehicles results from smog chamber experiments AtmosChem Phys 10 11545ndash11563

Choeumll M Deboudt K Flament P 2010 Development of time-resolveddescription of aerosol properties at the particle scale during an episodeof industrial pollution plume Water Air Soil Pollut 209 93ndash107

Christian TJ Yokelson RJ Caacuterdenas B Molina LT Engling G Hsu SC2010 Trace gas and particle emissions from domestic and industrialbiofuel use and garbage burning in central Mexico Atmos Chem Phys10 565ndash584

Chuang CC Penner JE Taylor KE Grossman AS Walton JJ 1997 Anassessment of the radiative effects of anthropogenic sulfate J GeophysRes 102 3761ndash3778

Claeys M Graham B Vas G Wang W Vermeylen R Pashynska VCafmeyer J Guyon P Andreae MO Artaxo P Maenhaut W 2004Formation of secondary organic aerosols through photooxidation ofisoprene Science 303 1173

Claeys M Wang W Vermeylen R Kourtchev I Chi X Farhat Y SurrattJD Goacutemez-Gonzaacutelez Y Sciare J Maenhaut W 2010 Chemicalcharacterisation of marine aerosol at Amsterdam Island during theaustral summer of 2006ndash2007 J Aerosol Sci 41 13ndash22

Cohen JB Ruston AG 1932 Smoke a Study of Town Air 4 E ArnoldLondon (1912 88 pp)

Collins E 1926 Tuberculosis-silicosis Brochure 32 Occupation and HealthInternational Labor Office Geneva p 62

Cook PA Savage NH Turquety S Carver GD OConnor FM Heckel AStewart D Whalley LK Parker AE Schlager H Singh HB Avery MASachse GW BruneW Richter A Burrows JP Purvis R Lewis AC ReevesCE Monks PS Levine JG Pyle JA 2007 Forest fire plumes over the North



Atlantic p-TOMCAT model simulations with aircraft and satellite measure-ments from the ITOPICARTT campaign J Geophys Res 112 (D10S43)

Cooray V Rahman M Rakov V 2009 On the NOx production by laboratoryelectrical discharges and lightning J Atmos Sol Terr Phys 71 1877ndash1889

Corbett JJ Fischbeck P 1997 Emissions from ships Science 278 823Corradini S Merucci L Prata AJ Piscini A 2010 Volcanic ash and SO2 in

the 2008 Kasatochi eruption retrievals comparison from different IRsatellite sensors J Geophys Res 115 (D00L21)

Costa EAL Campos VP Da Silva Filho LCP Greven HA 2009Evaluation of the aggressive potential of marine chloride and sulfatesalts on mortars applied as renders in the Metropolitan Region ofSalvador - Bahia Brazil J Environ Manage 90 1060ndash1068

Costner P 2006 Update of Dioxin Emission Factors for Forest FiresGrassland and Moor Fires Open Burning of Agricultural Residues OpenBurning of Domestic Waste Landfills and Dump Fires InternationalPOPs Elimination Network Mexico

Coulier P 1875 Note sur une nouvelle proprieteacute de lair J Pharm Chim 22165ndash173

Coz E Goacutemez-Moreno FJ Casuccio GS Artiacutentildeano B 2010 Variationson morphology and elemental composition of mineral dust particlesfrom local regional and long-range transport meteorological scenariosJ Geophys Res 115 D12204

Csavina J Landaacutezuri A Wonaschuumltz A Rine K Rheinheimer P Barbaris BConant W Saacuteez A Betterton E 2011 Metal andmetalloid contaminantsin atmospheric aerosols frommining operationsWater Air Soil Pollut 221145ndash157

Dahl A Gharibi A Swietlicki E Gudmundsson A BohgardM Ljungman ABlomqvist G GustafssonM 2006 Traffic-generated emissions of ultrafineparticles from pavementndashtire interface Atmos Environ 40 1314ndash1323

Danckelman V 1884 Die Bevoelkungsverhaeltnisse des suedwstlichenAfricas Meteorol Z 8 301ndash311

Das SK Jayaraman A 2012 Long-range transportation of anthropogenicaerosols over Eastern coastal region of India investigation of sourcesand impact on regional climate change Atmos Res 118 68ndash83

Davies CN 1966 Aerosol Science Academic Press (468 pp)De Bruijne K Ebersviller S Sexton K Lake S Leith D Goodman R

Jetters J Walters G Doyle-Eisele M Woodside R 2009 Design andtesting of electrostatic aerosol in vitro exposure system (EAVES) analternative exposure system for particles Inhal Toxicol 21 91ndash101

Delmas R Meacutegie G Peuch VH 2005 Physique et chimie de latmosphegravereBerlin

DeMott PJ Prenni AJ Liu X Kreidenweis SM Petters MD Twohy CHRichardson M Eidhammer T Rogers D 2010 Predicting globalatmospheric ice nuclei distributions and their impacts on climate ProcNatl Acad Sci U S A 107 11217

Dentener F Kinne S Bond T Boucher O Cofala J Generoso SGinoux P Gong S Hoelzemann JJ Ito A Marelli L Penner JEPutaud JP Textor C Schulz M Van Der Werf GR Wilson J 2006Emissions of primary aerosol and precursor gases in the years 2000and 1750 prescribed data-sets for AeroCom Atmos Chem Phys 64321ndash4344

Derbyshire E 2007 Natural minerogenic dust and human health Ambio 3673ndash77

Derevianko GJ Deutsch C Hall A 2009 On the relationship betweenocean DMS and solar radiation Geophys Res Lett 36 L17606

Deshler T 2008 A review of global stratospheric aerosol measurementsimportance life cycle and local stratospheric aerosol Atmos Res 90223ndash232

Despreacutes VR Huffman JA Burrows SM Hoose C Safatov AS Buryak GFroumlhlich-Nowoisky J Elbert W Andreae MO Poumlschl U Jaenicke R2012 Primary biological aerosol particles in the atmosphere a reviewTellus Ser B Chem Phys Meteorol 64 15598 httpdxdoiorg103402tellusbv64i015598

Dinkage LE 1891 Staubfaelle im Passatgebiet des NordatlantischenOceans Ann Hydrogr 19 313ndash318

Domingo JL Nadal M 2009 Domestic waste composting facilities areview of human health risks Environ Int 35 382ndash389

Donnelly JR 1992 Metal emissions control technologies for wasteincineration In khan MR (Ed) Clean Energy from Waste and CoalAmerican Chemical Society pp 174ndash188

Drinker P Hatch T 1936 Industrial dust hygienic significance measure-ment and control Third Impression First Edition McGraw-Hill BookCompany Inc (Hardcover 316 pp)

Drinker P Hatch T 1954 Industrial Dust McGraw-Hill (112 pp)Dron J Abidi E Haddad IE Marchand N Wortham H 2008 Precursor

ion scanning-mass spectrometry for the determination of nitro func-tional groups in atmospheric particulate organic matter Anal ChimActa 618 184ndash195

Duarte RMBO Santos EBH Pio CA Duarte AC 2007 Comparison ofstructural features of water-soluble organic matter from atmospheric

aerosols with those of aquatic humic substances Atmos Environ 418100ndash8113

Duggen S Olgun N Croot P Hoffmann L Dietze H Delmelle PTeschner C 2010 The role of airborne volcanic ash for the surface oceanbiogeochemical iron-cycle a review Biogeosciences 7 827ndash844

Durant AJ Bonadonna C Horwell CJ 2010 Atmospheric and environ-mental impacts of volcanic particulates Elements 6 235ndash240

Dusek U Frank GP Hildebrandt L Curtius J Schneider J Walter SChand D Drewnick F Hings S Jung D Borrmann S Andreae MO2006 Size matters more than chemistry for cloud-nucleating ability ofaerosol particles Science 312 1375ndash1378

EC 2004 Second Position Paper on Particulate Matter EuropeanCommission

Edwards RD Jurvelin J Saarela K Jantunen M 2001 VOC concentrationsmeasured in personal samples and residential indoor outdoor andworkplace microenvironments in EXPOLIS-Helsinki Finland AtmosEnviron 35 4531ndash4543

Egen PNC 1835 Der Haarrauch EssenEl Zein A Bedjanian Y 2012 Interaction of NO2 with TiO2 surface under UV

irradiation measurements of the uptake coefficient Atmos Chem Phys12 1013ndash1020

Elbert W Taylor P Andreae M Poumlschl U 2007 Contribution of fungi toprimary biogenic aerosols in the atmosphere wet and dry dischargedspores carbohydrates and inorganic ions Atmos Chem Phys 74569ndash4588

EPA 1996 Air Quality Criteria for Particulate Matter National Center forEnvironmental Assessment-RTP Office I

Fang GC Wu YS Rau JY Huang SH 2006 Traffic aerosols (18 nm leparticle size le 18 μm) source apportionment during the winter periodAtmos Res 80 294ndash308

Finessi E Decesari S Paglione M Giulianelli L Carbone C Gilardoni SFuzzi S Saarikoski S Raatikainen T Hillamo R Allan J Mentel TFTiitta P Laaksonen A Petaumljauml T Kulmala M Worsnop DR FacchiniMC 2012 Determination of the biogenic secondary organic aerosolfraction in the boreal forest by AMS and NMR measurements AtmosChem Phys 12 941ndash959

Finlayson-Pitts BJ Pitts Jr JN 1986 Atmospheric chemistry Fundamen-tals and Experimental Techniques John Wiley amp Sons Inc

Fisseha R Saurer M Jaggi M Szidat S Siegwolf RTW Baltensperger U2006 Determination of stable carbon isotopes of organic acids andcarbonaceous aerosols in the atmosphere Rapid Commun MassSpectrom 20 2343ndash2347

Flagan RC 1998 History of electrical aerosol measurements Aerosol SciTechnol 28 301ndash380

Flossmann AI Wobrock W 2010 A review of our understanding of theaerosolndashcloud interaction from the perspective of a bin resolved cloudscale modelling Atmos Res 97 478ndash497

Formenti P Elbert W Maenhaut W Haywood J Osborne S AndreaeMO 2003 Inorganic and carbonaceous aerosols during the SouthernAfrican Regional Science Initiative (SAFARI 2000) experiment chemicalcharacteristics physical properties and emission data for smoke fromAfrican biomass burning J Geophys Res 108 8488

Formenti P Schuetz L Balkanski Y Desboeufs K Ebert M Kandler KPetzold A Scheuvens D Weinbruch S Zhang D 2011 Recentprogress in understanding physical and chemical properties of mineraldust Atmos Chem Phys 11 8231ndash8256

Forster P Ramaswamy V Artaxo P Berntsen T Betts R Fahey DWHaywood J Lean J Lowe DC Myhre G Nganga J Prinn R Raga GSchulz M Dorland RV 2007 Changes in atmospheric constituents andin radiative forcing In Solomon S Qin D Manning M Chen ZMarquis M Averyt KB Tignor M Miller HL (Eds) Climate Change2007 The Physical Science Basis Contribution of Working Group I to theFourth Assessment Report of the Intergovernmental Panel on ClimateChange Cambridge University Press Cambridge United Kingdom andNew York NY USA

Franklin B 1784 Meteorological inaugurations and conjectures Mem LitPhilos Soc Manchester II 30

Fruin SA Winer AM Rodes CE 2004 Black carbon concentrations inCalifornia vehicles and estimation of in-vehicle diesel exhaust particu-late matter exposures Atmos Environ 38 4123ndash4133

Fuchs NA 1964 The Mechanics of Aerosols Pergamon Press OxfordFuzzi S Andreae MO Huebert BJ Kulmala M Bond TC Boy M

Doherty SJ Guenther A Kanakidou M Kawamura K KerminenVM Lohmann U Russell LM Poumlschl U 2006 Critical assessment ofthe current state of scientific knowledge terminology and researchneeds concerning the role of organic aerosols in the atmosphereclimate and global change Atmos Chem Phys 6 2017ndash2038

Gaffney JS Marley NA 2009 The impacts of combustion emissions on airquality and climate mdash from coal to biofuels and beyond Atmos Environ43 23ndash36



Ganzeveld LN Van Aardenne JA Butler TM Lawrence MG MetzgerSM Stier P Zimmermann P Lelieveld J 2006 Technical noteAnthropogenic and natural offline emissions and the online EMissionsand dry DEPosition submodel EMDEP of the Modular Earth Submodelsystem (MESSy) Atmos Chem Phys Discuss 6 5457ndash5483

Gao C Oman L Robock A Stenchikov GL 2007 Atmospheric volcanicloading derived from bipolar ice cores accounting for the spatialdistribution of volcanic deposition J Geophys Res 112 D09109

Garg BD Cadle SH Mulawa PA Groblicki PJ Laroo C Parr GA 2000 Brakewear particulate matter emissions Environ Sci Technol 34 4463ndash4469

Gebhart KA Malm WC Day D 1994 Examination of the effects of sulfateacidity and relative humidity on light scattering at Shenandoah NationalPark Atmos Environ 28 841ndash849

Gelencseacuter A May B Simpson D Saacutenchez-Ochoa A Kasper-Giebl APuxbaum H Caseiro A Pio C Legrand M 2007 Source apportionmentof PM25 organic aerosol over Europe primarysecondary naturalanthropogenic and fossilbiogenic origin J Geophys Res 112 (D23S04)

Gentry JW 1997 The legacy of John Tyndall in aerosol science J AerosolSci 28 1365ndash1372

Gilardoni S Vignati E Cavalli F Putaud J Larsen B Karl M Stenstroumlm KGenberg J Henne S Dentener F 2011 Better constraints on sources ofcarbonaceous aerosols using a combined 14C-macro tracer analysis in aEuropean rural background site Atmos Chem Phys 11 5685ndash5700

Ginoux P Garbuzov D Hsu NC 2010 Identification of anthropogenic andnatural dust sources usingModerate Resolution ImagingSpectroradiometer(MODIS) Deep Blue level 2 data J Geophys Res 115 D05204

Gonccedilalves C Alves C Evtyugina M Mirante F Pio C Caseiro A SchmidlC Bauer H Carvalho F 2010 Characterisation of PM10 emissions fromwoodstove combustion of common woods grown in Portugal AtmosEnviron 44 4474ndash4480

Gong W Dastoor AP Bouchet VS Gong S Makar PA Moran MDPabla B Meacutenard S Crevier LP Cousineau S Venkatesh S 2006Cloud processing of gases and aerosols in a regional air quality model(AURAMS) Atmos Res 82 248ndash275

Graf H-F Feichter J Langmann B 1997 Volcanic sulfur emissionsestimates of source strength and its contribution to the global sulfatedistribution J Geophys Res 102 10727ndash10738

Grini A Zender CS Colarco PR 2002 Saltation sandblasting behaviorduring mineral dust aerosol production Geophys Res Lett 29 1868

Guenther A Karl T Harley P Wiedinmyer C Palmer PI Geron C 2006Estimates of global terrestrial isoprene emissions using MEGAN (Modelof Emissions of Gases and Aerosols from Nature) Atmos Chem Phys 63181ndash3210

Guoliang C Xiaoye Z Sunling G Fangcheng Z 2008 Investigation onemission factors of particulate matter and gaseous pollutants from cropresidue burning J Environ Sci 20 50ndash55

Hallquist M Wenger JC Baltensperger U Rudich Y Simpson D Claeys MDommen J Donahue NM George C Goldstein AH Hamilton JFHerrmann H Hoffmann T Iinuma Y Jang M Jenkin ME Jimenez JLKiendler-Scharr A Maenhaut W Mcfiggans G Mentel TF Monod APreacutevocirct ASH Seinfeld JH Surratt JD Szmigielski R Wildt J 2009 Theformation properties and impact of secondary organic aerosol currentand emerging issues Atmos Chem Phys 9 5155ndash5236

Haywood J Boucher O 2000 Estimates of the direct and indirect radiativeforcing due to tropospheric aerosols a review Rev Geophys 38 513ndash543

Haywood JM Jones A Clarisse L Bourassa A Barnes J Telford PBellouin N Boucher O Agnew P Clerbaux C Coheur P DegensteinD Braesicke P 2010 Observations of the eruption of the Sarychevvolcano and simulations using the HadGEM2 climate model J GeophysRes 115 D21212

He L-Y Hu M Huang X-F Yu B-D Zhang Y-H Liu D-Q 2004Measurement of emissions of fine particulate organic matter fromChinese cooking Atmos Environ 38 6557ndash6564

Heald CL Spracklen DV 2009 Atmospheric budget of primary biologicalaerosol particles from fungal spores Geophys Res Lett 36 L09806

Hegg DA Livingston J Hobbs PV Novakov T Russell P 1997 Chemicalapportionment of aerosol column optical depth off the mid-Atlanticcoast of the United States J Geophys Res 102 25293ndash25303

Heintzenberg J 1985 What can we learn from aerosol measurements atbaseline stations J Atmos Chem 3 153ndash169

Henze DK Seinfeld JH 2006 Global secondary organic aerosol fromisoprene oxidation Geophys Res Lett 33 L09812

Hildemann LM Markowski GR Cass GR 1991 Chemical composition ofemissions from urban sources of fine organic aerosol Environ SciTechnol 25 744ndash759

Hjortenkrans DST Bergbaumlck BG Haumlggerud AV 2007 Metal emissionsfrom brake linings and tires case studies of Stockholm Sweden 19951998 and 2005 Environ Sci Technol 41 5224ndash5230

Holden AS Sullivan AP Munchak LA Kreidenweis SM Schichtel BAMalm WC Collett Jr JL 2011 Determining contributions of biomass

burning and other sources to fine particle contemporary carbon in thewestern United States Atmos Environ 45 1986ndash1993

Holmes NS Morawska L 2006 A review of dispersion modelling and itsapplication to the dispersion of particles an overview of differentdispersion models available Atmos Environ 40 5902ndash5928

Horwell C Baxter P 2006 The respiratory health hazards of volcanic ash areview for volcanic risk mitigation Bull Volcanol 69 1ndash24

Hoyle CR Boy M Donahue NM Fry JL Glasius M Guenther A HallarAG Huff Hartz K Petters MD Petaumljauml T Rosenoern T Sullivan AP2011 A review of the anthropogenic influence on biogenic secondaryorganic aerosol Atmos Chem Phys 11 321ndash343

Huang J Kang S Shen C Cong Z Liu K Wang W Liu L 2010 Seasonalvariations and sources of ambient fossil and biogenic-derived carbona-ceous aerosols based on 14C measurements in Lhasa Tibet Atmos Res96 553ndash559

Huang C Chen CH Li L Cheng Z Wang HL Huang HY Streets DGWang YJ Zhang GF Chen YR 2011 Emission inventory ofanthropogenic air pollutants and VOC species in the Yangtze RiverDelta region China Atmos Chem Phys 11 4105ndash4120

Hungershoefer K Zeromskiene K Iinuma Y Helas G Trentmann JTrautmann T Parmar RS Wiedensohler A Andreae MO Schmid O2008 Modelling the optical properties of fresh biomass burning aerosolproduced in a smoke chamber results from the EFEU campaign AtmosChem Phys 8 3427ndash3439

Husar RB 2000 Atmospheric aerosol science before 1900 In Preining ODavis EJ (Eds) History of Aerosol Science Proceedings of theSymposium on the History of Aerosol Science Vienna Austria August31ndashSeptember 2 1999 Verlag der Oesterreichischen Akademie derWissenschaften Wien pp 25ndash36

Iijima A Sato K Yano K Tago H Kato M Kimura H Furuta N 2007Particle size and composition distribution analysis of automotive brakeabrasion dusts for the evaluation of antimony sources of airborneparticulate matter Atmos Environ 41 4908ndash4919

Iinuma Y Engling G Puxbaum H Herrmann H 2009 A highly resolvedanion-exchange chromatographic method for determination of saccaridictracers for biomass combustion and primary bio-particles in atmosphericaerosol Atmos Environ 43 1367ndash1371

Ilyinskaya E Oppenheimer C Mather TA Martin RS Kyle PR 2010Size-resolved chemical composition of aerosol emitted by Erebusvolcano Antarctica Geochem Geophys Geosyst 11 Q03017

IPCC 2007 The physical science basis Contribution of Working Group I tothe Fourth Assessment Report of the Intergovernmental Panel onClimate Change Cambridge University Press Cambridge United King-dom and New York NY USA p 996

Iwamoto Y Yumimoto K Toratani M Tsuda A Miura K Uno IUematsu M 2011 Biogeochemical implications of increased mineralparticle concentrations in surface waters of the northwestern NorthPacific during an Asian dust event Geophys Res Lett 38 L01604

Jacobson MZ 2001 Global direct radiative forcing due to multi-component anthropogenic and natural aerosols J Geophys Res 1061551ndash1568

Jacobson MC Hansson HC Noone KJ Charlson RJ 2000 Organicatmospheric aerosols review and state of the science Rev Geophys 38267ndash294

Jaenicke R 2005 Abundance of cellular material and proteins in theatmosphere Science 308 73

Jang HN Seo YC Lee JH Hwang KW Yoo JI Sok CH Kim SH 2007Formation of fine particles enriched by V and Ni from heavy oilcombustion anthropogenic sources and drop-tube furnace experi-ments Atmos Environ 41 1053ndash1063

Janhaumlll S Andreae MO Poumlschl U 2010 Biomass burning aerosolemissions from vegetation fires particle number and mass emissionfactors and size distributions Atmos Chem Phys 10 1427ndash1439

Jankowski N Schmidl C Marr IL Bauer H Puxbaum H 2008Comparison of methods for the quantification of carbonate carbon inatmospheric PM10 aerosol samples Atmos Environ 42 8055ndash8064

Jiang M Marr LC Dunlea EJ Herndon SC Jayne JT Kolb CE KnightonWB Rogers TM Zavala M Molina LT Molina MJ 2005 Vehicle fleetemissions of black carbon polycyclic aromatic hydrocarbons and otherpollutants measured by a mobile laboratory in Mexico City Atmos ChemPhys 5 3377ndash3387

Johansson LS Tullin C Leckner B Sjoumlvall P 2003 Particle emissions frombiomass combustion in small combustors Biomass Bioenergy 25 435ndash446

Kar SK Liou YA Ha KJ 2009 Aerosol effects on the enhancement ofcloud-to-ground lightning over major urban areas of South KoreaAtmos Res 92 80ndash87

Karanasiou A Diapouli E Cavalli F Eleftheriadis K Viana M Alastuey AQuerol X Reche C 2011 On the quantification of atmospheric carbonatecarbon by thermaloptical analysis protocols Atmos Meas Tech 42409ndash2419



Katul GG Groumlnholm T Launiainen S Vesala T 2011 The effects of thecanopy medium on dry deposition velocities of aerosol particles in thecanopy sub-layer above forested ecosystems Atmos Environ 451203ndash1212

Kempf N 1914 Die Entwicklung der Theorien uumlber den HoumlhenrauchDoctors Dissertation vor der Kgl Technischen Hochschule zu MuenchenVerlag von FCW Vogel

Kerker M 1997 Light scattering instrumentation for aerosol studies anhistorical overview Aerosol Sci Technol 27 522ndash540

Khain A Cohen N Lynn B Pokrovsky A 2008 Possible aerosol effects onlightning activity and structure of hurricanes J Atmos Sci 65 3652ndash3677

Khalil MAK Rasmussen RA 2003 Tracers of wood smoke AtmosEnviron 37 1211ndash1222

Kiessling J 1888 Untersuch ueber Daemmerungs-Erscheing zur Erklaerungd nach d Krakatauausbrush beobact atmosphaer Opstich Stoerung

Kim MK Kennicutt MC Qian YR 2005 Polycyclic aromatic hydrocarbonpurification procedures for compound specific isotope analysis EnvironSci Technol 39 6770ndash6776

Kim JH Yum SS Lee Y-G Choi B-C 2009 Ship measurements ofsubmicron aerosol size distributions over the Yellow Sea and the EastChina Sea Atmos Res 93 700ndash714

Kittelson DB 1998 Engines and nanoparticles a review J Aerosol Sci 29575ndash588

Klaver A Formenti P Caquineau S Chevaillier S Ausset P Calzolai GOsborne S Johnson B Harrison M Dubovik O 2011 Physico-chemicaland optical properties of Sahelian and Saharan mineral dust in situmeasurements during the GERBILS campaign Q J R Meteorol Soc 1371193ndash1210

Kleeman MJ Schauer JJ Cass GR 1999 Size and compositiondistribution of fine particulate matter emitted from wood burningmeat charbroiling and cigarettes Environ Sci Technol 33 3516ndash3523

Kleindienst TE Jaoui M Lewandowski M Offenberg JH Lewis CWBhave PV Edney EO 2007 Estimates of the contributions of biogenicand anthropogenic hydrocarbons to secondary organic aerosol at asoutheastern US location Atmos Environ 41 8288ndash8300

Kluumlser L Holzer-Popp T 2010 Mineral dust effects on clouds and rainfall inthe West African Sahel Atmos Chem Phys 10 6901ndash6915

Knaapen AM Borm PJ Albrecht C Schins RP 2004 Inhaled particlesand lung cancer Part A mechanisms J Int Cancer 109 799ndash809

Knobelspiesse K Cairns B Ottaviani M Ferrare R Hair J Hostetler CObland M Rogers R Redemann J Shinozuka Y Clarke A Freitag SHowell S Kapustin V Mcnaughton C 2011 Combined retrievals ofboreal forest fire aerosol properties with a polarimeter and Lidar AtmosChem Phys 11 7045ndash7067

Koch D Bond TC Streets D Unger N Van Der Werf GR 2007Global impacts of aerosols from particular source regions and sectorsJ Geophys Res 112 D02205

Koch D Bauer SE Del Genio A Faluvegi G Mcconnell JR Menon SMiller RL Rind D Ruedy R Schmidt GA Shindell D 2011 Coupledaerosolndashchemistryndashclimate twentieth-century transient model investi-gation trends in short-lived species and climate responses J Climate 242693ndash2714

Kok JF 2011a Does the size distribution of mineral dust aerosols dependon the wind speed at emission Atmos Chem Phys 11 10149ndash10156

Kok JF 2011b A scaling theory for the size distribution of emitted dustaerosols suggests climate models underestimate the size of the globaldust cycle Proc Natl Acad Sci U S A 108 1016ndash1021

Koppmann R Von Czapiewski K Reid JS 2005 A review of biomassburning emissions part I gaseous emissions of carbon monoxidemethane volatile organic compounds and nitrogen containing com-pounds Atmos Chem Phys Discuss 5 10455ndash10516

Kroll JH Seinfeld JH 2008 Chemistry of secondary organic aerosolformation and evolution of low-volatility organics in the atmosphereAtmos Environ 42 3593ndash3624

Kroll JH Ng NL Murphy SM Flagan RC Seinfeld JH 2006 Secondaryorganic aerosol formation from isoprene photooxidation Environ SciTechnol 40 1869ndash1877

Kulmala M Vehkamaumlki H Petaumljauml T Dal Maso M Lauri A KerminenVM Birmili W Mcmurry PH 2004 Formation and growth rates ofultrafine atmospheric particles a review of observations J Aerosol Sci35 143ndash176

Kulmala M Asmi A Lappalainen HK Baltensperger U Brenguier JLFacchini MC Hansson HC Hov Oslash ODowd CD Poumlschl UWiedensohler A Boers R Boucher O De Leeuw G Denier Van DerGon HAC Feichter J Krejci R Laj P Lihavainen H Lohmann UMcfiggans G Mentel T Pilinis C Riipinen I Schulz M Stohl ASwietlicki E Vignati E Alves C Amann M Ammann M Arabas SArtaxo P Baars H Beddows DCS Bergstroumlm R Beukes JP Bilde MBurkhart JF Canonaco F Clegg SL Coe H Crumeyrolle S DAnna BDecesari S Gilardoni S Fischer M Fjaeraa AM Fountoukis C

George C Gomes L Halloran P Hamburger T Harrison RMHerrmann H Hoffmann T Hoose C Hu M Hyvaumlrinen A HotilderrakU Iinuma Y Iversen T Josipovic M Kanakidou M Kiendler-ScharrA Kirkevaringg A Kiss G Klimont Z Kolmonen P Komppula MKristjaacutensson JE Laakso L Laaksonen A Labonnote L Lanz VALehtinen KEJ Rizzo LV Makkonen R Manninen HE McmeekingG Merikanto J Minikin A Mirme S Morgan WT Nemitz EODonnell D Panwar TS Pawlowska H Petzold A Pienaar JJ Pio CPlass-Duelmer C Preacutevocirct ASH Pryor S Reddington CL Roberts GRosenfeld D Schwarz J Seland Oslash Sellegri K Shen XJ Shiraiwa MSiebert H Sierau B Simpson D Sun JY Topping D Tunved PVaattovaara P Vakkari V Veefkind JP Visschedijk A Vuollekoski HVuolo R Wehner B Wildt J Woodward S Worsnop DR vanZadelhoff GJ Zardini AA Zhang K van Zyl PG Kerminen VMCarslaw KS Pandis SN 2011 General overview European Integratedproject on Aerosol Cloud Climate and Air Quality interactions (EUCAARI)mdashintegrating aerosol research fromnano to global scales Atmos Chem Phys11 13061ndash13143

Kupiainen KJ Tervahattu H Raumlisaumlnen M Maumlkelauml T Aurela M HillamoR 2004 Size and composition of airborne particles from pavementwear tires and traction sanding Environ Sci Technol 39 699ndash706

Lack D Lerner B Granier C Massoli P Baynard T Lovejoy ERavishankara A Williams E 2007 Light absorbing carbon emissionsfrom commercial shipping impacts for local air quality and the ArcticEOS Transactions American Geophysical Union Fall Meeting SupplAbstract A32A-05

Lai ACK Chen FZ 2007 Modeling of cooking-emitted particle dispersionand deposition in a residential flat a real room application BuildEnviron 42 3253ndash3260

Lana A Bell TG Simoacute R Vallina SM Ballabrera-Poy J Kettle AJ Dachs JBopp L Saltzman ES Stefels J Johnson JE Liss PS 2011 An updatedclimatology of surface dimethylsulfide concentrations and emission fluxesin the global ocean Global Biogeochem Cycles 25 (GB1004)

Langmann B Zakšek K Hort M Duggen S 2010 Volcanic ash as fertiliserfor the surface ocean Atmos Chem Phys 10 3891ndash3899

Lau APS Lee AKY Chan CK Fang M 2006 Ergosterol as a biomarkerfor the quantification of the fungal biomass in atmospheric aerosolsAtmos Environ 40 249ndash259

Lemieux PM Lutes CC Abbott JA Aldous KM 2000 Emissions ofpolychlorinated dibenzo-p-dioxins and polychlorinated dibenzofuransfrom the open burning of household waste in barrels Environ SciTechnol 34 377ndash384

Lemieux PM Gullett BK Lutes CC Winterrowd CK Winters DL 2003Variables affecting emissions of PCDDFs from uncontrolled combustionof household waste in barrels J Air Waste Manage Assoc 53 523ndash531

Levin Z Cotton WR 2008 Aerosol Pollution Impact on Precipitation AScientific Review Geneva SwitzerlandWorldMeteorological OrganizationReport from the WMOIUGG International Aerosol Precipitation ScienceAssessment Group (IAPSAG) World Meteorological Organization GenevaSwitzerland

Li Z Zhao X Kahn R Mishchenko M Remer L Lee KH Wang MLaszlo I Nakajima T Maring H 2009 Uncertainties in satellite remotesensing of aerosols and impact on monitoring its long-term trend areview and perspective Ann Geophys 27 2755ndash2770

Li QWangW Zhang HWWang YJ Wang B Li L Li HJWang BJ ZhanJ Wu M Bi XH 2010 Development of a compound-specific carbonisotope analysis method for 2-methyltetrols biomarkers for secondaryorganic aerosols from atmospheric isoprene Anal Chem 82 6764ndash6769

Li PH Han B Huo J Lu B Ding X Chen L Kong SF Bai ZP Wang B2012a Characterization meteorological influences and source identifi-cation of carbonaceous aerosols during the autumnndashwinter period inTianjin China Aerosol Air Qual Res 12 283ndash294

LiW Shi Z Zhang D Zhang X Li P Feng Q Yuan QWangW 2012bHazeparticles over a coal-burning region in the China Loess Plateau in winterthree flight missions in December 2010 J Geophys Res 117 D12306

Liao H Seinfeld JH 2005 Global impacts of gas-phase chemistryndashaerosolinteractions on direct radiative forcing by anthropogenic aerosols andozone J Geophys Res 110 D18208

Liao H Chen WT Seinfeld JH 2006 Role of climate change in globalpredictions of future tropospheric ozone and aerosols J Geophys Res111 D12304

Lin YF Wu YPG Chang CT 2007 Combustion characteristics of waste-oil produced biodieseldiesel fuel blends Fuel 86 1772ndash1780

Linak WP Yoo JI Wasson SJ Zhu W Wendt JO Huggins FE Chen YShah N Huffman GP Gilmour MI 2007 Ultrafine ash aerosols fromcoal combustion characterization and health effects Proc CombustInst 31 1929ndash1937

Liu G Niu Z Van Niekerk D Xue J Zheng L 2008 Polycyclic aromatichydrocarbons (PAHs) from coal combustion emissions analysis andtoxicology Rev Environ Contam Toxicol 192 1ndash28



Liu Z Ge Y Johnson KC Shah AN Tan J Wang C Yu L 2011 Real-world operation conditions and on-road emissions of Beijing dieselbuses measured by using portable emission measurement system andelectric low-pressure impactor Sci Total Environ 409 1476ndash1480

Lobert JM Keene WC Logan JA Yevich R 1999 Global chlorineemissions from biomass burning reactive chlorine emissions inventoryJ Geophys Res 104 8373ndash8389

Lodge JP Evelyn J Barr R 1969 The Smoke of London Maxwell ReprintCo New York

Loeb NG Su W 2010 Direct aerosol radiative forcing uncertainty based ona radiative perturbation analysis J Climate 23 5288ndash5293

Lohmann U Feichter J 2005 Global indirect aerosol effects a reviewAtmos Chem Phys 5 715ndash737

Lohmann U Leck C 2005 Importance of submicron surface-active organicaerosols for pristine Arctic clouds Tellus Ser B Chem Phys Meteorol 57261ndash268

Long CM Suh HH Koutrakis P 2000 Characterization of indoor particlesources using continuous mass and size monitors J Air Waste Manage50 1236ndash1250

Lorenzo R Kaegi R Gehrig R Grobeacutety B 2006 Particle emissions of arailway line determined by detailed single particle analysis AtmosEnviron 40 7831ndash7841

Lukaacutecs H Gelencseacuter A Hoffer A Kiss G Horvaacuteth K Hartyaacuteni Z 2009Quantitative assessment of organosulfates in size-segregated rural fineaerosol Atmos Chem Phys 9 231ndash238

Ma S Peng PA Song J Zhao J He L Sheng G Fu J 2010 Stable carbonisotopic compositions of organic acids in total suspended particles anddusts from Guangzhou China Atmos Res 98 176ndash182

MacGorman DR Rust WD 1998 The Electrical Nature of Storms OxfordUniversity Press USA (422 pp)

Mahowald NM Kloster S Engelstaedter S Moore JK Mukhopadhyay SMcconnell JR Albani S Doney SC Bhattacharya A Curran MaJFlanner MG Hoffman FM Lawrence DM Lindsay K Mayewski PANeff J Rothenberg D Thomas E Thornton PE Zender CS 2010Observed 20th century desert dust variability impact on climate andbiogeochemistry Atmos Chem Phys 10 10875ndash10893

Mahowald N Lindsay K Rothenberg D Doney SC Moore JK ThorntonP Randersn JT Jones CD 2011a Desert dust and anthropogenicaerosol interactions in the community climate system model coupled-carbon-climate model Biogeosciences 8 387ndash414

Mahowald N Ward DS Kloster S Flanner MG Heald CL HeavensNG Hess PG Lamarque JF Chuang PY 2011b Aerosol impacts onclimate and biogeochemistry Annu Rev Environ Resour 36 45ndash74

Marmer E Langmann B 2005 Impact of ship emissions on theMediterranean summertime pollution and climate a regional modelstudy Atmos Environ 39 4659ndash4669

Martuzevicius D Grinshpun SA Lee T Hu S Biswas P Reponen TLemasters G 2008 Traffic-related PM25 aerosol in residential houseslocated near major highways indoor versus outdoor concentrationsAtmos Environ 42 6575ndash6585

Mason RP 2009 Mercury fate and transport in the global atmosphereIn Mason R Pirrone N (Eds) Mercury Emissions from NaturalProcesses and Their Importance in the Global Mercury Cycle SpringerUS pp 173ndash191

Mather TA Pyle DM Oppenheimer C 2003 Tropospheric volcanic aerosolIn Robock A Oppenheimer C (Eds) Volcanism and the EarthsAtmosphere Volcanism and the Earths Atmosphere AGUWashingtonDC

McCubbin DR Apelberg BJ Roe S Divita F 2002 Livestock ammoniamanagement and particulate mdash related health benefits Environ SciTechnol 36 1141ndash1146

McDonald JD Zielinska B Fujita EM Sagebiel JC Chow JC WatsonJG 2003 Emissions from charbroiling and grilling of chicken and beefJ Air Waste Manage Assoc 53 185ndash194

McMeeking GR Kreidenweis SM Baker S Carrico CM Chow JCCollett Jr JL Hao WM Holden AS Kirchstetter TW Malm WCMoosmuumlller H Sullivan AP Wold CE 2009 Emissions of trace gasesand aerosols during the open combustion of biomass in the laboratoryJ Geophys Res 114 D19210

McMurdo CJ Ellis DA Webster E Butler J Christensen RD Reid LK2008 Aerosol enrichment of the surfactant PFO and mediation of thewaterndashair transport of gaseous PFOA Environ Sci Technol 42 3969ndash3974

McMurry PH 2000a The history of condensation nucleus counters AerosolSci Technol 33 297ndash322

McMurry PH 2000b A review of atmospheric aerosol measurementsAtmos Environ 34 1959ndash1999

Meacuteszaacuteros E 1999 Fundamentals of Atmospheric Aerosol ChemistryAkadeacutemiai Kiado Budapest

Meacuteszaacuteros A Vissy K 1974 Concentration size distribution and chemicalnature of atmospheric aerosol particles in remote oceanic areas J AerosolSci 5 101ndash109

Mijic Z Rajšic S Perišic AŽM Stojic A Tasic M 2010 Characteristicsand application of receptor models to the atmospheric aerosols researchIn Kumar A (Ed) Air quality pp 143ndash167

Minguilloacuten BMC 2007 Composicioacuten y fuentes del material particuladoatmosfeacuterico en la zona ceraacutemica de Castelloacuten Impacto de la introduccioacutende las Mejores Teacutecnicas Disponibles PhD Thesis Universitat Jaume I(Barcelona)

Miracolo MA Hennigan CJ Ranjan M Nguyen NT Gordon TD LipskyEM Presto AA Donahue NM Robinson AL 2011 Secondary aerosolformation from photochemical aging of aircraft exhaust in a smogchamber Atmos Chem Phys 11 4135ndash4147

Miranda J Zepeda F Galindo I 2004 The possible influence of volcanicemissions on atmospheric aerosols in the city of Colima MexicoEnviron Pollut 127 271ndash279

Mishchenko MI 2010 Review of satellite aerosol remote sensing over land InKokhanovsky AA de Leeuw G (Eds) J Quant Radiat Transfer 111 p 259

Miyazaki Y Kawamura K Sawano M 2010 Size distributions of organicnitrogen and carbon in remote marine aerosols evidence of marinebiological origin based on their isotopic ratios Geophys Res Lett 37L06803

Mohr C Huffman JA Cubison MJ Aiken AC Docherty KS Kimmel JRUlbrich IM Hannigan M Jimenez JL 2009 Characterization ofprimary organic aerosol emissions from meat cooking trash burningand motor vehicles with high-resolution aerosol mass spectrometryand comparison with ambient and chamber observations Environ SciTechnol 43 2443ndash2449

Moumlnkkoumlnen P Koponen I Lehtinen K Uma R Srinivasan D Haumlmeri KKulmala M 2004 Death of nucleation and Aitken mode particlesobservations at extreme atmospheric conditions and their theoreticalexplanation J Aerosol Sci 35 781ndash787

Monks PS Granier C Fuzzi S Stohl A Williams ML Akimoto HAmann M Baklanov A Baltensperger U Bey I Blake N Blake RSCarslaw K Cooper OR Dentener F Fowler D Fragkou E Frost GJGeneroso S Ginoux P Grewe V Guenther A Hansson HC HenneS Hjorth J Hofzumahaus A Huntrieser H Isaksen ISA Jenkin MEKaiser J Kanakidou M Klimont Z Kulmala M Laj P Lawrence MGLee JD Liousse C Maione M Mcfiggans G Metzger A Mieville AMoussiopoulos N Orlando JJ ODowd CD Palmer PI Parrish DDPetzold A Platt U Poumlschl U Preacutevocirct ASH Reeves CE Reimann SRudich Y Sellegri K Steinbrecher R Simpson D Ten Brink HTheloke J Van Der Werf GR Vautard R Vestreng V Vlachokostas CVon Glasow R 2009 Atmospheric composition change mdash global andregional air quality Atmos Environ 43 5268ndash5350

Moosmuumlller H Gillies J Rogers C Dubois D Chow J Watson JLangston R 1998 Particulate emission rates for unpaved shouldersalong a paved road J Air Waste Manage Assoc 48 398ndash407

Moreno T Querol X Alastuey A GibbonsW 2009 Identification of chemicaltracers in the characterisation and source apportionment of inhalableinorganic airborne particles an overview Biomarkers 14 17ndash22

Moreno T Querol X Alastuey A Amato F Pey J Pandolfi M Kuenzli NBouso L Rivera M Gibbons W 2010 Effect of fireworks events onurban background trace metal aerosol concentrations is the cocktailworth the show J Hazard Mater 183 945ndash949

Morrical BD Zenobi R 2002 Determination of aromatic tracer compoundsfor environmental tobacco smoke aerosol by two step laser massspectrometry Atmos Environ 36 801ndash811

Mulitza S Heslop D Pittauerova D Fischer HW Meyer I Stuut JBZabel M Mollenhauer G Collins JA Kuhnert H 2010 Increase inAfrican dust flux at the onset of commercial agriculture in the Sahelregion Nature 466 226ndash228

Myhre G Grini A Metzger S 2006 Modelling of nitrate and ammonium-containing aerosols in presence of sea salt Atmos Chem Phys 6 4809ndash4821

Napier F Darcy B Jefferies C 2008 A review of vehicle related metals andpolycyclic aromatic hydrocarbons in the UK environment Desalination226 143ndash150

Ndour M Danna B George C Ka O Balkanski Y Kleffmann JStemmler K Ammann M 2008 Photoenhanced uptake of NO2 onmineral dust laboratory experiments and model simulations GeophysRes Lett 35 L05812

Nilsson ED Paatero J Boy M 2001a Effects of air masses and synopticweather on aerosol formation in the continental boundary layer TellusSer B Chem Phys Meteorol 53 462ndash478

Nilsson ED Rannik Uuml Kumala M Buzorius G Dowd CD 2001b Effects ofcontinental boundary layer evolution convection turbulence and entrain-ment on aerosol formation Tellus Ser B Chem Phys Meteorol 53 441ndash461

Novakov T Penner JE 1993 Large contribution of organic aerosols tocloudndashcondensationndashnuclei concentrations Nature 365 823ndash826

ODonnell D Tsigaridis K Feichter J 2011 Estimating the direct andindirect effects of secondary organic aerosols using ECHAM5-HAMAtmos Chem Phys 11 8635ndash8659



ODowd CD Langmann B Varghese S Scannell C Ceburnis D FacchiniMC 2008 A combined organicndashinorganic sea-spray source functionGeophys Res Lett 35 L01801

Oros DR Simoneit BRT 2001a Identification and emission factors ofmolecular tracers in organic aerosols from biomass burning part 1temperate climate conifers Appl Geochem 16 1513ndash1544

Oros DR Simoneit BRT 2001b Identification and emission factors ofmolecular tracers in organic aerosols from biomass burning part 2deciduous trees Appl Geochem 16 1545ndash1565

Oros DR Abas MRB Omar NYMJ Rahman NA Simoneit BRT 2006Identification and emission factors of molecular tracers in organicaerosols from biomass burning part 3 grasses Appl Geochem 21919ndash940

Ortiz De Zaacuterate I Ezcurra A Lacaux JP Van Dinh P 2000 Emission factorestimates of cereal waste burning in Spain Atmos Environ 343183ndash3193

Ortiz De Zaacuterate I Ezcurra A Lacaux JP Van Dinh P De Argandontildea JD2005 Pollution by cereal waste burning in Spain Atmos Res 73161ndash170

Pacyna JM 1998 Source inventories for atmospheric trace metals InHarrison RM Van Grieken RE (Eds) Atmospheric particles IUPACSeries on Analytical and Physical Chemistry of Environmental Systemsvol 5 Wiley pp 387ndash423

Pan Y-L Pinnick RG Hill SC Rosen JM Chang RK 2007 Single-particlelaser-induced-fluorescence spectra of biological and other organic-carbonaerosols in the atmosphere measurements at New Haven Connecticutand Las Cruces New Mexico J Geophys Res 112 (D24S19)

Pang X Lewis AC 2011 Carbonyl compounds in gas and particle phases ofmainstream cigarette smoke Sci Total Environ 409 5000ndash5009

Park SS Bae MS Schauer JJ Ryu SY Kim YJ Yong Cho S Kim SJ2005 Evaluation of the TMO and TOT methods for OC and ECmeasurements and their characteristics in PM25 at an urban site ofKorea during ACE-Asia Atmos Environ 39 5101ndash5112

Park RJ Kim MJ Jeong JI Youn D Kim S 2010 A contribution of browncarbon aerosol to the aerosol light absorption and its radiative forcing inEast Asia Atmos Environ 44 1414ndash1421

Pathak RK Wu WS Wang T 2009 Summertime PM25 ionic species infour major cities of China nitrate formation in an ammonia-deficientatmosphere Atmos Chem Phys 9 1711ndash1722

Penner J 1995 Carbonaceous aerosols influencing atmospheric radiationblack and organic carbon In Charlson RJ Heintzenberg J (Eds)Aerosol Forcing of Climate John Wiley and Sons Chichester pp 91ndash108

Penner JEEA 2001 Aerosols their direct and indirect effects InHoughton JT et al (Ed) Climate Change 2001 The Scientific BasisContribution of Working Group I to the Third Assessment Report of theIntergovernmental Panel on Climate Change Cambridge UniversityPress Cambridge United Kingdom and New York NY USA pp 289ndash348

Pentildeuelas J Llusiagrave J 2001 The complexity of factors driving volatile organiccompound emissions by plants Biol Platarum 44 481ndash487

Peacutereacute JC Mallet M Pont V Bessagnet B 2011 Impact of aerosol directradiative forcing on the radiative budget surface heat fluxes andatmospheric dynamics during the heat wave of summer 2003 overwestern Europe a modeling study J Geophys Res 116 D23119

Pinder RW Davidson EA Goodale CL Greaver TL Herrick JD Liu L2012 Climate change impacts of US reactive nitrogen Proc Natl AcadSci U S A 109 (20) 7671ndash7675

Pio C Cerqueira M Harrison RM Nunes T Mirante F Alves C OliveiraC Sanchez De La Campa A Artiacutentildeano B Matos M 2011 OCEC ratioobservations in Europe re-thinking the approach for apportionmentbetween primary and secondary organic carbon Atmos Environ 456121ndash6132

Pirrone N Cinnirella S Feng X Finkelman RB Friedli HR Leaner JMason R Mukherjee AB Stracher GB Streets DG Telmer K 2010Global mercury emissions to the atmosphere from anthropogenic andnatural sources Atmos Chem Phys 10 5951ndash5964

Plotkin SE 2007 Examining fuel economy and carbon standards for lightvehicles Discussion Paper No 2007-1 International Transport Forum

Podzimek J 1989 John Aitkens contribution to atmospheric and aerosolsciences in hundred years of condensation nuclei counting Bull AmMeteorol Soc 70 1538ndash1545

Podzimek J Cartens JC 1985 The 100 year evolution of Aitken nucleicounters current and future problems J Rech Atmosph 19 257ndash274

Poumlschl U 2005 Atmospheric aerosols composition transformation climateand health effects Angew Chem Int Ed 44 7520ndash7540

Poacutesfai M Molnaacuter A 2000 Aerosol particles in the troposphere amineralogical introduction EMU Notes Mineral 2 197ndash252

Prata A Tupper A 2009 Aviation hazards from volcanoes the state of thescience Nat Hazards 51 239ndash244

Preining O 1996 The many facets of aerosol science J Aerosol Sci 27(Suppl 1) S1ndashS6

Prestel MAF 1861 Meteorologische Untersuchungen betreffend dieVerbreitung des Moorrauchs den Tagen vom 20 Bis 26 Mai 1860 dieisobarometrischen Linien am 22 Mai und die Gewitter am 20 Und 26Mai 1860 Kleine Schrifte der Naturforschenden Geselschaft in EmdenEmden Schnellpressen Druck von Th Hahn Wwe Emden

Prichard HM Fisher PC 2012 Identification of platinum and palladiumparticles emitted from vehicles and dispersed into the surface environ-ment Environ Sci Technol 46 3149ndash3154

Prospero JM Ginoux P Torres O Nicholson SE Gill TE 2002Environmental characterization of global sources of atmospheric soildust identified with the NIMBUS 7 Total Ozone Mapping Spectrometer(TOMS) absorbing aerosol product Rev Geophys 40 1002

Prospero JM Blades E Mathison G Naidu R 2005 Interhemispherictransport of viable fungi and bacteria from Africa to the Caribbean withsoil dust Aerobiologia 21 1ndash19

Putaud JP Van Dingenen R Alastuey A Bauer H Birmili W Cyrys JFlentje H Fuzzi S Gehrig R Hansson HC Harrison RM HerrmannH Hitzenberger R Huumlglin C Jones AM Kasper-Giebl A Kiss GKousa A Kuhlbusch TAJ LOumlschau G Maenhaut W Molnar AMoreno T Pekkanen J Perrino C Pitz M Puxbaum H Querol XRodriguez S Salma I Schwarz J Smolik J Schneider J Spindler Gten Brink H Tursic J Viana M Wiedensohler A Raes F 2010 AEuropean aerosol phenomenology mdash 3 physical and chemical charac-teristics of particulate matter from 60 rural urban and kerbside sitesacross Europe Atmos Environ 44 1308ndash1320

Puxbaum H Tenze-Kunit M 2003 Size distribution and seasonal variationof atmospheric cellulose Atmos Environ 37 3693ndash3699

Querol X Alastuey A Puicercus JA Mantilla E Miro JV Lopez-Soler APlana F Artintildeano B 1998a Seasonal evolution of suspended particlesaround a large coal-fired power station particulate levels and sourcesAtmos Environ 32 1963ndash1978

Querol X Alastuey AS Puicercus JA Mantilla E Ruiz CR Lopez-SolerA Plana F Juan R 1998b Seasonal evolution of suspended particlesaround a large coal-fired power station chemical characterizationAtmos Environ 32 719ndash731

Querol X Alastuey A Rodriacuteguez S Plana F Mantilla E Ruiz CR 2001Monitoring of PM10 and PM25 around primary particulate anthropo-genic emission sources Atmos Environ 35 845ndash858

Querol X Alastuey A Ruiz CR Artintildeano B Hansson HC Harrison RMBuringh E Ten Brink HM Lutz M Bruckmann P Straehl PSchneider J 2004 Speciation and origin of PM10 and PM25 in selectedEuropean cities Atmos Environ 38 6547ndash6555

Querol X Alastuey A Pey J Cusack M Peacuterez N Mihalopoulos NTheodosi C Gerasopoulos E Kubilay N Koccedilak M 2009a Variabilityin regional background aerosols within the Mediterranean AtmosChem Phys 9 4575ndash4591

Querol X Pey J Pandolfi M Alastuey A Cusack M Peacuterez N Moreno TViana M Mihalopoulos N Kallos G Kleanthous S 2009b Africandust contributions to mean ambient PM10 mass-levels across theMediterranean Basin Atmos Environ 43 4266ndash4277

Quinn PK Miller TL Bates TS Ogren JA Andrews E Shaw GE 2002A 3-year record of simultaneously measured aerosol chemical andoptical properties at Barrow Alaska J Geophys Res 107 4130

Quinn PK Bates TS Baum E Doubleday N Fiore AM Flanner MFridlind A Garrett TJ Koch D Menon S Shindell D Stohl AWarren SG 2008 Short-lived pollutants in the Arctic their climateimpact and possible mitigation strategies Atmos Chem Phys 81723ndash1735

Radke LF Hegg DA Hobbs PV Nance JD Lyons JH Laursen KKWeiss RE Riggan PJ Ward DE 1991 Particulate and trace gasemission from large biomass fires in North America In Levine JS (Ed)Global Biomass Burning MIT Press pp 209ndash224

Rafinesque C 1819 Thoughts on atmospheric dust Am J Sci I (4)Rafinesque C 1820 Anonymous correspondent ldquoXYZrdquo of Boston reply to

Rafinesque Sillimans Am J 2 134ndash135Ravindra K Mor S Kaushik CP 2003 Short-term variation in air quality

associated with firework events a case study J Environ Monit 5260ndash264

Redmond HE Dial KD Thompson JE 2010 Light scattering andabsorption by wind blown dust theory measurement and recentdata Aeolian Res 2 5ndash26

Reemtsma T These A Venkatachari P Xia X Hopke PK Springer ALinscheid M 2006 Identification of fulvic acids and sulfated andnitrated analogues in atmospheric aerosol by electrospray ionizationFourier transform ion cyclotron resonance mass spectrometry AnalChem 78 8299ndash8304

Reid JS Eck TF Christopher SA Koppmann R Dubovik O EleuterioDP Holben BN Reid EA Zhang J 2005a A review of biomassburning emissions part III intensive optical properties of biomassburning particles Atmos Chem Phys 5 827ndash849



Reid JS Koppmann R Eck TF Eleuterio DP 2005b A review of biomassburning emissions part II intensive physical properties of biomassburning particles Atmos Chem Phys 5 799ndash825

Revuelta MA Sastre M Fernaacutendez AJ Martiacuten L Garciacutea R Goacutemez-Moreno FJ Artiacutentildeano B Pujadas M Molero F 2012 Characterizationof the Eyjafjallajoumlkull volcanic plume over the Iberian Peninsula by Lidarremote sensing and ground-level data collection Atmos Environ 4846ndash55

Richard A Gianini MFD Mohr C Furger M Bukowiecki N MinguilloacutenMC Lienemann P Flechsig U Appel K Decarlo PF Heringa MFChirico R Baltensperger U Preacutevocirct ASH 2011 Source apportionmentof size and time resolved trace elements and organic aerosols from anurban courtyard site in Switzerland Atmos Chem Phys 11 8945ndash8963

Roberts TJ Braban CF Martin RS Oppenheimer C Adams JW CoxRA Jones RL Griffiths PT 2009 Modelling reactive halogenformation and ozone depletion in volcanic plumes Chem Geol 263151ndash163

Robinson AL Subramanian R Donahue NM Bernardo-Bricker A RoggeWF 2006 Source apportionment of molecular markers and organicaerosol 3 Food cooking emissions Environ Sci Technol 40 7820ndash7827

Robock A 2000 Volcanic eruptions and climate Rev Geophys 38 191ndash219Roelofs G 2008 A GCM study of organic matter in marine aerosol and its

potential contribution to cloud drop activation Atmos Chem Phys 8709ndash719

Rogge WF Hildemann LM Mazurek MA Cass GR Simoneit BRT1991 Sources of fine organic aerosol 1 Charbroilers and meat cookingoperations Environ Sci Technol 25 1112ndash1125

Rogge WF Hildemann LM Mazurek MA Cass GR Simoneit BRT1993 Sources of fine organic aerosol 3 Road dust tire debris andorganometallic brake lining dust roads as sources and sinks EnvironSci Technol 27 1892ndash1904

Rogge WF Hildemann LM Mazurek MA Cass GR Simoneit BRT1994 Sources of fine organic aerosol 6 Cigarette smoke in the urbanatmosphere Environ Sci Technol 28 1375ndash1388

Ryu SY Kwon BG Kim YJ Kim HH Chun KJ 2007 Characteristics ofbiomass burning aerosol and its impact on regional air quality in thesummer of 2003 at Gwangju Korea Atmos Res 84 362ndash373

Saacutenchez de la Campa AM de La Rosa JD Gonzaacutelez-Castanedo YFernaacutendez-Camacho R Alastuey A Querol X Pio C 2010 Highconcentrations of heavy metals in PM from ceramic factories of SouthernSpain Atmos Res 96 633ndash644

Sanders PG Xu N Dalka TM Maricq MM 2003 Airborne brake weardebris size distributions composition and a comparison of dynamom-eter and vehicle tests Environ Sci Technol 37 4060ndash4069

Schaap M Spindler G Schulz M Acker K Maenhaut W Berner AWieprecht W Streit N Muumlller K Bruumlggemann E Chi X Putaud JPHitzenberger R Puxbaum H Baltensperger U Ten Brink H 2004Artefacts in the sampling of nitrate studied in the ldquoINTERCOMPrdquocampaigns of EUROTRAC-AEROSOL Atmos Environ 38 6487ndash6496

Schauer JJ Kleeman MJ Cass GR Simoneit BRT 2001 Measurement ofemissions from air pollution sources 4 C1ndashC27 organic compounds fromcooking with seed oils Environ Sci Technol 36 567ndash575

Schleicher NJ Norra S Chai F Chen Y Wang S Cen K Yu Y Stuumlben D2011 Temporal variability of trace metal mobility of urban particulatematter from Beijing mdash a contribution to health impact assessments ofaerosols Atmos Environ 45 7248ndash7265

Schmauss A 1920a Die chemie des nebels der wolken und des regens DieUnschau (FrankfurM Germany) 24 pp 61ndash63

Schmauss A 1920b Kolloidchemie und Meteorologie Metorologie 37 1ndash18Schmidl C Marr IL Caseiro A Kotianovaacute P Berner A Bauer H Kasper-

Giebl A Puxbaum H 2008 Chemical characterisation of fine particleemissions from wood stove combustion of common woods growing inmid-European Alpine regions Atmos Environ 42 126ndash141

Schumann U Huntrieser H 2007 The global lightning-induced nitrogenoxides source Atmos Chem Phys 7 3823ndash3907

See SW Balasubramanian R 2006 Physical characteristics of ultrafineparticles emitted from different gas cooking methods Aerosol Air QualRes 6 82ndash92

See SW Balasubramanian R 2008 Chemical characteristics of fineparticles emitted from different gas cooking methods Atmos Environ42 8852ndash8862

Seinfeld JH Pandis SN 1998 Atmospheric chemistry and physics AirPollution to Climate Change Wiley New York (1360 pp)

Seinfeld JH Pandis SN 2006 Atmospheric Chemistry and Physics From AirPollution to Climate Change 2nd Edition John Wiley amp Sons New York

Sellegri K 2002 Etude du processus dactivation des gouttelettes de nuageimplications en chimie multiphases PhD thesis Joseph Fourier Univer-sity Grenoble France

Sellegri K ODowd C Yoon Y Jennings S De Leeuw G 2006 Surfactantsand submicron sea spray generation J Geophys Res 111 D22215

Shank L Howell S Clarke A Freitag S Brekhovskikh V Kapustin VMcnaughton C Campos T Wood R 2012 Organic matter and non-refractory aerosol over the remote Southeast Pacific oceanic andcombustion sources Atmos Chem Phys 12 557ndash576

Shao Y Raupach M Findlater P 1993 Effect of saltation bombardment onthe entrainment of dust by wind J Geophys Res 98 (12719ndash12726)

Shen G Wang W Yang Y Zhu C Min Y Xue M Ding J Li W Wang BShen H Wang R Wang X Tao S 2010 Emission factors andparticulate matter size distribution of polycyclic aromatic hydrocarbonsfrom residential coal combustions in rural Northern China AtmosEnviron 44 5237ndash5243

Shi Y Zhang N Gao J Li X Cai Y 2011 Effect of fireworks display onperchlorate in air aerosols during the Spring Festival Atmos Environ 451323ndash1327

Shindell D Faluvegi G 2009 Climate response to regional radiative forcingduring the twentieth century Nat Geosci 2 294ndash300

Shindell D Faluvegi G 2010 The net climate impact of coal-fired powerplant emissions Atmos Chem Phys 10 3247ndash3260

Sigerson G 1870 Micro-atmospheric researches Proc Roy Irish Acad 1 13ndash31Simoneit BRT 2002 Biomass burning mdash a review of organic tracers for

smoke from incomplete combustion Appl Geochem 17 129ndash162Sinclair D 1950 Handbook on Aerosols Atomic Energy Commission

Washington DCSingh RB Sloan JJ 2006 A high-resolution NOx emission factor model for

North American motor vehicles Atmos Environ 40 5214ndash5223Sjaastad AK 2010 Exposure to cooking fumes during the pan frying of

beefsteak under domestic and occupational conditions PhD ThesisNorwegian University of Science and Technology

Skeie RB Fuglestvedt J Berntsen T Lund MT Myhre G Rypdal K2009 Global temperature change from the transport sectors historicaldevelopment and future scenarios Atmos Environ 43 6260ndash6270

Skeie RB Berntsen T Myhre G Pedersen CA Stroumlm J Gerland SOgren JA 2011 Black carbon in the atmosphere and snow from pre-industrial times until present Atmos Chem Phys 11 6809ndash6836

Smith SJ Van Aardenne J Klimont Z Andres RJ Volke A Delgado AriasS 2011 Anthropogenic sulfur dioxide emissions 1850ndash2005 AtmosChem Phys 11 1101ndash1116

Spurny KR 1993 Aerosol science of the early days J Aerosol Sci 24 S1ndashS2Spurny KR 1998 Methods of aerosol measurement before the 1960s

Aerosol Sci Technol 29 329ndash349Spurny KR 2000 Atmospheric condensation nuclei P J Coulier 1875 and J

Aitken 1880 (Historical Review) Aerosol Sci Technol 32 243ndash248Spurny KR 2001 Historical aspects of aerosols measurements In Baron

PA Willeke K (Eds) Aerosols Measurement Principles Techniquesand Applications 2nd ed John Wiley amp Sons Inc New York pp 3ndash30

Squizzato S Masiol M Brunelli A Pistollato S Tarabotti E Rampazzo GPavoni B 2012 Factors determining the formation of secondaryinorganic aerosol a case study in the Po Valley (Italy) Atmos ChemPhys Discuss 12 16377ndash16406

Starik A 2008 Gaseous and particulate emissions with jet engine exhaustand atmospheric pollution Advances on Propulsion Technology forHigh-Speed Aircraft (pp 15-1ndash15-22) Educational Notes RTO-EN-AVT-150 Paper 15 Neuilly-sur-Seine RTO France

Stelson AW Seinfeld JH 1981 Chemical mass accounting of urbanaerosol Environ Sci Technol 15 671ndash679

Stern DI 2006 Reversal of the trend in global anthropogenic sulfuremissions Glob Environ Change 16 207ndash220

Stohl A Prata AJ Eckhardt S Clarisse L Durant A Henne S KristiansenNI Minikin A Schumann U Seibert P Stebel K Thomas HEThorsteinsson T Toslashrseth K Weinzierl B 2011 Determination of time-and height-resolved volcanic ash emissions and their use for quantitativeash dispersion modeling the 2010 Eyjafjallajoumlkull eruption Atmos ChemPhys 11 4333ndash4351

Szidat S Jenk TM Synal H-A Kalberer M Wacker L Hajdas I Kasper-Giebl A Baltensperger U 2006 Contributions of fossil fuel biomass-burning and biogenic emissions to carbonaceous aerosols in Zurich astraced by 14C J Geophys Res 111 D07206

Tafuro AM Barnaba F De Tomasi F Perrone MR Gobbi GP 2006Saharan dust particle properties over the central Mediterranean AtmosRes 81 67ndash93

Talhout R Schulz T Florek E Van Benthem J Wester P Opperhuizen A2011 Hazardous compounds in tobacco smoke Int J Environ ResPublic Health 8 613ndash628

Tan Z Tay R 2008 Sources contributing to PM25 in a commercial truckcabin in winter Transp Res D 13 54ndash58

Tegen I Werner M Harrison SP Kohfeld KE 2004 Relative importanceof climate and land use in determining present and future global soildust emission Geophys Res Lett 31 L05105

Thevenon F Chiaradia M Adatte T Hueglin C Poteacute J 2011 Ancientversus modern mineral dust transported to high-altitude Alpine glaciers



evidences Saharan sources and atmospheric circulation changes AtmosChem Phys 11 859ndash884

Thomas HE Watson IM Kearney C Carn SA Murray SJ 2009 A multi-sensor comparison of sulphur dioxide emissions from the 2005 eruptionof Sierra Negra volcano Galaacutepagos Islands Remote Sens Environ 1131331ndash1342

Thorpe A Harrison RM 2008 Sources and properties of non-exhaustparticulate matter from road traffic a review Sci Total Environ 400270ndash282

Tohka A Karvosenoja N 2006 Fine Particle Emissions and EmissionReduction Potential in Finnish Industrial Processes Reports of FinnishEnvironment Institute

Trang TTD Byeong-Kyu L 2011 Determining contamination level ofheavy metals in road dust from busy traffic areas with differentcharacteristics J Environ Manage 92 554ndash562

Trochkine D Iwasaka Y Matsuki A Yamada M Kim YS Nagatani TZhang D Shi GY Shen Z 2003 Mineral aerosol particles collected inDunhuang China and their comparison with chemically modifiedparticles collected over Japan J Geophys Res 108 8642

Tsai J-H Chiang H-L Hsu Y-C Peng B-J Hung R-F 2005 Developmentof a local real world driving cycle for motorcycles for emission factormeasurements Atmos Environ 39 6631ndash6641

Tsitouridou R Anatolaki C 2007 On the wet and dry deposition of ionicspecies in the vicinity of coal-fired power plants northwestern GreeceAtmos Res 83 93ndash105

Tunved P Korhonen H Stroumlm J Hansson HC Lehtinen KEJ KulmalaM 2004 A pseudo-Lagrangian model study of the size distributionproperties over Scandinavia transport from Aspvreten to VaumlarrioumlAtmos Chem Phys Discuss 4 7757ndash7794

Turekian VC Macko SA Keene WC 2003 Concentrations isotopiccompositions and sources of size-resolved particulate organic carbonand oxalate in near-surface marine air at Bermuda during springJ Geophys Res 108 4157

Turpin BJ Lim H-J 2001 Species contributions to PM25mass concentrationsrevisiting common assumptions for estimating organic mass Aerosol SciTechnol 35 602ndash610

Tyndall J 1871 On dust and smoke The Royal Institute Library of Science(TRILS-ps) 2 pp 302ndash313

Udden JA 1896 Dust and sand storms in the West Pop Sci Mon 44655ndash664

Urbanski S Hao W Nordgren B 2011 The wildland fire emissioninventory western United States emission estimates and an evaluationof uncertainty Atmos Chem Phys 11 12973ndash13000

USEPA 2006 An inventory of sources and environmental releases of dioxin-like compounds in the United States for the years 1987 1995 and 2000EPA600P-03002F National Center for Environmental AssessmentOffice of Research and Development Washington DC p 677

Van DerWerf GR Randerson JT Giglio L Collatz G Mu M Kasibhatla PSMorton DC Defries R Jin Y Van Leeuwen TT 2010 Global fireemissions and the contribution of deforestation savanna forest agricul-tural and peat fires (1997ndash2009) Atmos Chem Phys 10 11707ndash11735

Vergaz R 2001 Propiedades oacutepticas de los aerosoles atmosfeacutericosCaracterizacioacuten del aacuterea del Golfo de Caacutediz PhD Thesis University ofValladolid Spain

Vernier JP Thomason LW Pommereau JP Bourassa A Pelon J GarnierA Hauchecorne A Blanot L Trepte C Degenstein D Vargas F 2011Major influence of tropical volcanic eruptions on the stratosphericaerosol layer during the last decade Geophys Res Lett 38 L12807

Viana M Kuhlbusch TaJ Querol X Alastuey A Harrison RM Hopke PKWiniwarter W Vallius M Szidat S Preacutevocirct ASH Hueglin C BloemenH Waringhlin P Vecchi R Miranda AI Kasper-Giebl A Maenhaut WHitzenberger R 2008 Source apportionment of particulate matter inEurope a review of methods and results J Aerosol Sci 39 827ndash849

Vignati E Facchini MC Rinaldi M Scannell C Ceburnis D Sciare JKanakidou M Myriokefalitakis S Dentener F ODowd CD 2010Global scale emission and distribution of sea-spray aerosol sea-salt andorganic enrichment Atmos Environ 44 670ndash677

Wainwright M Wickramasinghe N Narlikar J Rajaratnam P 2003Microorganisms cultured from stratospheric air samples obtained at41 km FEMS Microbiol Lett 218 161ndash165

Walton WH 1982 The nature hazards and assessment of occupationalexposure to airborne asbestos dust a review Ann Occup Hyg 25 117ndash119

Walton WH Vincent JH 1998 Aerosol instrumentation in occupationalhygiene an historical perspective Aerosol Sci Technol 28 417ndash438

Wang H Kawamura K 2006 Stable carbon isotopic composition of low-molecular-weight dicarboxylic acids and ketoacids in remote marineaerosols J Geophys Res 111 D07304

Wang H Kawamura K Yamazaki K 2006 Water-soluble dicarboxylicacids ketoacids and dicarbonyls in the atmospheric aerosols over thesouthern ocean and western pacific ocean J Atmos Chem 53 43ndash61

Wang J Hoffmann AA Park RJ Jacob DJ Martin ST 2008 Globaldistribution of solid and aqueous sulfate aerosols effect of the hysteresisof particle phase transitions J Geophys Res 113 D11206

Wang M Ghan S Easter R Ovchinnikov M Liu X Kassianov E Qian YGustafson Jr W Larson V Schanen D 2011a The multi-scale aerosol-climate model PNNL-MMF model description and evaluation GeosciModel Dev 4 137ndash168

Wang Q Jacob D Fisher J Mao J Leibensperger E Carouge C Le SagerP Kondo Y Jimenez J Cubison M 2011b Sources of carbonaceousaerosols and deposited black carbon in the Arctic in winterndashspringimplications for radiative forcing Atmos Chem Phys 11 12453ndash12473

Wang Y Wan Q Meng W Liao F Tan H Zhang R 2011c Long-termimpacts of aerosols on precipitation and lightning over the Pearl RiverDelta megacity area in China Atmos Chem Phys 11 12421ndash12436

Warneck P 1988 Chemistry of the Natural Atmosphere Academic PressLondon

Warneke C De Gouw JA Del Negro L Brioude J Mckeen S Stark HKuster WC Goldan PD Trainer M Fehsenfeld FC Wiedinmyer CGuenther AB Hansel A Wisthaler A Atlas E Holloway JS RyersonTB Peischl J Huey LG Hanks ATC 2010 Biogenic emissionmeasurement and inventories determination of biogenic emissions inthe eastern United States and Texas and comparison with biogenicemission inventories J Geophys Res 115 (D00F18)

Washington R Todd MC 2005 Atmospheric controls on mineral dustemission from the Bodeacuteleacute Depression Chad the role of the low level jetGeophys Res Lett 32 L17701

Watanabe M Iwasaka Y Shibata T Hayashi M Fujiwara M Neuber R2004 The evolution of Pinatubo aerosols in the Arctic stratosphereduring 1994ndash2000 Atmos Res 69 199ndash215

Watson JG Chow JC Fujita EM 2001 Review of volatile organiccompound source apportionment by chemical mass balance AtmosEnviron 35 1567ndash1584

Whelpdale DM Dorling SR Hicks BB Summers PW 1996 Atmospher-ic process In Whelpdale DM Kaiser MS (Eds) Global aciddeposition assessment Report Number 106 World MeteorologicalOrganization Global Atmosphere Watch Geneva pp 7ndash32

White WH 2008 Chemical markers for sea salt in IMPROVE aerosol dataAtmos Environ 42 261ndash274

Widory D Roy S Le Moullec Y Goupil G Cocherie A Guerrot C 2004The origin of atmospheric particles in Paris a view through carbon andlead isotopes Atmos Environ 38 953ndash961

Winiwarter W Bauer H Caseiro A Puxbaum H 2009 Quantifyingemissions of primary biological aerosol particle mass in Europe AtmosEnviron 43 1403ndash1409

Witsaman RJ Comstock RD Smith GA 2006 Pediatric fireworks-relatedinjuries in the United States 1990ndash2003 Pediatrics 118 296ndash303

Womiloju TO Miller JD Mayer PM Brook JR 2003 Methods todetermine the biological composition of particulate matter collectedfrom outdoor air Atmos Environ 37 4335ndash4344

Woodcock AH 1972 Smaller salt particles in oceanic air and bubblebehavior in the sea J Geophys Res 77 5316ndash5321

Xu M Yu D Yao H Liu X Qiao Y 2011 Coal combustion-generatedaerosols formation and properties P Combust Inst 33 1681ndash1697

Yang M Howell S Zhuang J Huebert B 2009 Attribution of aerosol lightabsorption to black carbon brown carbon and dust in Chinamdashinterpretations of atmospheric measurements during EAST-AIREAtmos Chem Phys 9 2035ndash2050

Yang GP Zhang HH Zhou LM Yang J 2011 Temporal and spatial variationsof dimethylsulfide (DMS) and dimethylsulfoniopropionate (DMSP) in theEast China Sea and the Yellow Sea Cont Shelf Res 31 1325ndash1335

Yokelson R Burling I Urbanski S Atlas E Adachi K Buseck PWiedinmyer C Akagi S Toohey D Wold C 2011 Trace gas andparticle emissions from open biomass burning in Mexico Atmos ChemPhys 11 6787ndash6808

Yu F 2011 A secondary organic aerosol formation model consideringsuccessive oxidation aging and kinetic condensation of organic compoundsglobal scale implications Atmos Chem Phys 11 1083ndash1099

Yu F Turco RP 2001 From molecular clusters to nanoparticles role ofambient ionization in tropospheric aerosol formation J Geophys Res106 4797ndash4814

Yuan CS Lee CG Liu SH Chang JC Yuan C Yang HY 2006Correlation of atmospheric visibility with chemical composition ofKaohsiung aerosols Atmos Res 82 663ndash679

Yuan T Remer LA Pickering KE Yu H 2011 Observational evidence ofaerosol enhancement of lightning activity and convective invigorationGeophys Res Lett 38 L04701

Zeuthen JH Pedersen AJ Hansen J Frandsen FJ Livbjerg H RiberC Astrup T 2007 Combustion aerosols from municipal wasteincineration mdash effect of fuel feedstock and plant operation CombustSci Technol 179 2171ndash2198



Zhang Q 2005 Study on Regional Fine PM Emissions and Modeling inChina Tsinghua University China Beijing (in Chinese)

Zhang Q Jimenez JL Canagaratna MR Allan JD Coe H Ulbrich IAlfarra MR Takami A Middlebrook AM Sun YL Dzepina KDunlea E Docherty K Decarlo PF Salcedo D Onasch T Jayne JTMiyoshi T Shimono A Hatakeyama S Takegawa N Kondo YSchneider J Drewnick F Borrmann S Weimer S Demerjian KWilliams P Bower K Bahreini R Cottrell L Griffin RJ Rautiainen JSun JY Zhang YM Worsnop DR 2007 Ubiquity and dominance ofoxygenated species in organic aerosols in anthropogenically-influencedNorthern Hemisphere midlatitudes Geophys Res Lett 34 L13801

Zhang Y Schauer JJ Zhang Y Zeng L Wei Y Liu Y Shao M 2008Characteristics of particulate carbon emissions from real-world Chinesecoal combustion Environ Sci Technol 42 5068ndash5073

Zhang LW Bai ZP You Y Wu JH Feng YC Zhu T 2009a Chemicaland stable carbon isotopic characterization for PAHs in aerosol emittedfrom two indoor sources Chemosphere 75 453ndash461

Zhang Y Wang X Chen H Yang X Chen J Allen JO 2009b Sourceapportionment of lead-containing aerosol particles in Shanghai usingsingle particle mass spectrometry Chemosphere 74 501ndash507

Zhang M Wang X Chen J Cheng T Wang T Yang X Gong Y Geng FChen C 2010a Physical characterization of aerosol particles during theChinese New Years firework events Atmos Environ 44 5191ndash5198

Zhang R Shen Z Cheng T Zhang M Liu Y 2010b The elementalcomposition of atmospheric particles at Beijing during Asian dust eventsin spring 2004 Aerosol Air Qual Res 10 67ndash75

Zhang X Jiang H Jin J Xu X Zhang Q 2012 Analysis of acid rainpatterns in northeastern China using a decision tree method AtmosEnviron 46 590ndash596

Zhao Y Hu M Slanina S Zhang Y 2006 Chemical compositions of fineparticulate organic matter emitted from Chinese cooking Environ SciTechnol 41 99ndash105



Research on aerosol sources and chemical composition Past current andemerging issues

AI Calvo a C Alves a A Castro b V Pont c AM Vicente a R Fraile b

a Centre for Environmental and Marine Studies (CESAM) University of Aveiro 3810-193 Aveiro Portugalb Department of Physics IMARENAB University of Leoacuten 24071 Leoacuten Spainc Laboratoire dAeacuterologieOMP UMR 5560 Universiteacute de Toulouse III CNRS-UPS 14 av E Belin 31400 Toulouse France

a r t i c l e i n f o a b s t r a c t

Article historyReceived 23 April 2012Received in revised form 12 September 2012Accepted 15 September 2012

In spite of considerable progresses in recent years a quantitative and predictive understanding ofatmospheric aerosol sources chemical composition transformation processes and environmentaleffects is still rather limited and therefore represents a major research challenge in atmosphericscience This review begins with a historical perspective on the scientific questions regardingatmospheric aerosols over the past centuries followed by a description of the distributionsources transformation processes and chemical and physical properties as they are currentlyunderstood The major open questions and suggestions for future research priorities are outlinedto narrow the gap between the present understanding of the contribution of both anthropogenicand biogenic aerosols to radiative forcing resulting from the spatial non-uniformity intermittencyof sources unresolved composition and reactivity

copy 2012 Elsevier BV All rights reserved

KeywordsAerosolsHistorical aspectsChemical compositionSourcesResearch perspectives

Contents

1 Introduction and scope of the review 02 History of aerosol science 03 Aerosol chemical composition main sources 0

31 Main aerosol sources 0311 Anthropogenic sources 0312 Natural sources 0

32 The chemical composition of aerosols 0321 Sulphur species 0322 Nitrogen species 0323 Carbonaceous species 0

4 Suggestions for further research 05 Concluding remarks 0Acknowledgments 0Appendix A Supplementary data 0References 0

1 Introduction and scope of the review

Today there is a growing interest in improving air qualityby both the general public and individual governments This

Atmospheric Research 120ndash121 (2013) 1ndash28

Corresponding authorE-mail address anacalvouapt (AI Calvo)

0169-8095$ ndash see front matter copy 2012 Elsevier BV All rights reservedhttpdxdoiorg101016jatmosres201209021

Contents lists available at SciVerse ScienceDirect

Atmospheric Research

j ourna l homepage wwwe lsev ie r com locate atmos



















































Primary Secondary




Biomassburning



In-cloudprocessing





Levoglucosan

HULIS



minus NH4+




2minus


2minus and NO3minus


minus



























































312 Natural sources



























































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References



















































































































































































































































































































































































































































































































Primary Secondary




Biomassburning



In-cloudprocessing





Levoglucosan

HULIS



minus NH4+




2minus


2minus and NO3minus


minus



























































312 Natural sources



























































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References





































































































































































































































































































































































































































































































Primary Secondary




Biomassburning



In-cloudprocessing





Levoglucosan

HULIS



minus NH4+




2minus


2minus and NO3minus


minus



























































312 Natural sources



























































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References






















































































































































































































































































































































































































































































Primary Secondary




Biomassburning



In-cloudprocessing





Levoglucosan

HULIS



minus NH4+




2minus


2minus and NO3minus


minus



























































312 Natural sources



























































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References






































































































































































































































































































































































































































































Primary Secondary




Biomassburning



In-cloudprocessing





Levoglucosan

HULIS



minus NH4+




2minus


2minus and NO3minus


minus



























































312 Natural sources



























































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References

























































































































































































































































































































































































































































































































312 Natural sources



























































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References











































































































































































































































































































































































































































































































312 Natural sources



























































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References



























































































































































































































































































































































































































































































312 Natural sources



























































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References















































































































































































































































































































































































































































































312 Natural sources



























































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References



































































































































































































































































































































































































































































312 Natural sources



























































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References












































































































































































































































































































































































































































































































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References





























































































































































































































































































































































































































































































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References















































































































































































































































































































































































































































































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References

























































































































































































































































































































































































































































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References















































































































































































































































































































































































































































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References





































































































































































































































































































































































































































































Useless instrument

One

cla

ss

Few

cla

sses

Man

y cl

asse

s

Cla

sses

to

spec

ies

Mol

ecul

arid

enti

fica

tion

OCEC100

80

60

40

20

0


PILS-OC

FTIR

NMR

VUV

PBTDMS

HR-AMS

CI EA

2D-GC-MS

GC-MS

LC-MS

Com

plet

enes

s (

of

mas

s an

alys

ed)

Selectivity

HR-ToF-AMS
























Acknowledgments




References





















































































































































































































































































































































































































































































Acknowledgments




References












































































































































































































































































































































































































































































Acknowledgments




References





































































































































































































































































































































































































































































Acknowledgments




References























































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































































Documents

Research on aerosol sources and chemical composition: Past, current and emerging issues