7Be, 210Pb, and 210Po in the surface air from the Arctic to Antarctica

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Journal of Environmental Radioactivity xxx (2014) 1e11

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Journal of Environmental Radioactivity

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7Be, 210Pb, and 210Po in the surface air from the Arctic to Antarctica

Bertil R.R. Persson a,*,1, Elis Holm b

aMedical Radiation Physics, Lund University, Barngatan 2, SE 22185, Lund, SwedenbDepartment of radiation physics, Sahlgren Academy at the University of Gothenburg, SE 413 45 Gothenburg, Sweden

a r t i c l e i n f o

Article history:Received 30 March 2013Received in revised form16 December 2013Accepted 15 January 2014Available online xxx

Keywords:7Be210Pb210PoAtmosphereArcticAntarctica

* Corresponding author. Tel.: þ46 46173110; mobilE-mail address: [email protected] (B.R.R.

1 http://www.radfys.lu.se/b-persson/index.html.

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a b s t r a c t

In the present study we have investigated the activity concentrations of 210Pb, 210Po as well as 7Be insurface air of the North and South Atlantic (1988e1989), the Arctic Ocean (1991), and along the coastlineof Siberia (1994) during succeeding expeditions in the Swedish Polar Research program.

During the cruises in the Arctic Ocean during 1991-07-28 to 1991-10-04 the average air concentrationsof 7Be was 0.6 � 0.4 mBq/m3, 210Pb 40 � 4 mBq/m3 and 210Po-38 � 10 mBq/m3. During the Swedish-Russian Tundra Ecology-94 expedition along the Siberian coastline the average air concentrations of7Be and 210Pb measured during MayeJuly were 11 � 3, and 2.4 � 0.4 mBq/m3, and during JulyeSep-tember they were 7.2 � 2 and 2.7 � 1.1 mBq/m3 respectively. The results from measurements of theactivity concentration of 210Pb in the air over the Arctic Ocean vary between 75 and 176 mBq/m3. In the airclose to land masses, however, the activity concentration of 210Pb in the air increases to 269e2712 mBq/m3.

The activity concentration of 7Be in the South Atlantic during the cruise down to Antarctica variedbetween 1.3 and 1.7 with an average of 1.5 � 0.8 mBq/m3. The activity concentration of 210Pb in the SouthAtlantic down to Antarctica varied between 6 and 14 mBq/m3. At the Equator the activity concentrationrecorded in November 1988 was 630 mBq/m3 and in April 1989 it was 260 mBq/m3. The average activityconcentration of 210Pb during the route GothenburgeMontevideo in 1988 was 290 and on the returnMontevideoeGothenburg it was 230 mBq/m3. The activity concentration of 210Po in the South Atlanticdown to Antarctica varied between 15 and 58 mBq/m3. At the Equator the activity concentration inNovember 1988 was 170 and in April 1989 it was 70 mBq/m3. The average activity concentration of 210Poduring the route GothenburgeMontevideo in 1988 was 63 and on the return MontevideoeGothenburg itwas 60 mBq/m3. The average of the activity concentrations in the Antarctic air of 210Pb was 27 � 10 mBq/m3 and of 210Po it was 12 � 7 mBq/m3.

All our results were compiled together with other published data, and the global latitudinal distri-bution of 210Pb was converted to total annual deposition (Bq/m2/a) and fitted to a 4th degree polynomial.By using the global latitudinal distribution of 210Po/210Pb-activity ratio from our own results the globallatitudinal distribution of 210Po annual deposition was derived.

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1. Introduction

1.1. The natural origin of 210Pb and 210Po

The radioactive isotopes Lead-210 (210Pb) and Polonium-210(210Po) are produced in nature as a result of the decay of 238U andits daughters. The chain of decays until Radon-222 takes place inthe ground or in water deposits containing uranium:

e: þ46 708278087.Persson).

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238U > 234Th > 234Pa > 234U > 230Th > 226Ra > 222Rn(3.82 d)>

Radon-222 diffuses partly from the earth’s crust to the atmo-sphere where its concentration decreases monotony by height.222Rn decays with a half-life of 3.82 days to the following shortlived radon daughters:

>218Po (RaA 3.10 min) > 214Pb (RaB 26.8 min) > 214Bi(RaC 19.9 min) > 214Po (RaC0164.3 ms).

In the atmosphere the decay products from 222Rn attach toairborne particles and deposit as dry and wet deposition onto theearth’s surface. The decay products following 214Po are thefollowing long lived radio-nuclides and finally stable Lead-206:

nd 210Po in the surface air from the Arctic to Antarctica, Journal of014.01.008

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210Pb (RaD 22.20 a) > 210Bi (RaE 5.01 d) > 210Po(RaF 138.4 d) > 206Pb (stable).

The final radioactive isotope in the decay chain is 210Po with aspecific activity of 0.166 GBq/mg (166$1012 Bq/g ¼ 0.166$109 Bq/mg).

Radon-222 is exhaled from the ground at a rate of 18 mBq/m2/sor 48$1018 Bq per year (48 EBq/a) which confers the atmospheric210Pb at a rate of 23$1015 Bq/a (23 PBq/a) (Persson, 1970b). Thesource of 210Pb in the stratosphere is the emerging air at theequator which carries not only 210Pb but also 222Rn and itsdaughter-products, from which 210Pb and 210Po will be formed. Inthe vicinity of the tropopause the air concentration of 210Pb in-creases sharply (Burton and Stuart, 1960). The annual precipitation210Pb varies from a few Bq/m2 in the Antarctic to several hundredBq/m2 over large land masses (El-Daoushy, 1988; Eldaoushy andGarciatenorio, 1988; Roos et al., 1994). The amount of 210Pb-depo-sition depends on the surrounding surface of the earth and thepossibilities for exhalation of 222Rn. In urban areas release fromcoal-fired power plants also contribute to 210Po in the atmosphere(Abu Bakar et al., 2013; Alam and Mohamed, 2011; Baeza et al.,2012; Yan et al., 2012). The exhalation over sea, however, is smalldue to the low concentration of 226Ra in sea water which is onlyabout 1e2 mBq/l. The annual deposition of 210Pb in central Swedenwas estimated to about 63 Bq/m2/a (Persson, 1970a). Further out inthe Arctic ocean the depositional flux of 210Pb around Longitude154�W (150e156) is estimated to be around 16e22 Bq/m2/a, asextrapolated from published data (Baskaran and Naidu, 1995).

1.2. The natural origin of 7Be

Beryllium-7 is a natural radionuclide produced in the upper at-mosphere through spallation of oxygen and nitrogen nuclei by cos-mic rays. The use of 7Be as a tracer for the transport of aerosols in theatmosphere has been extensively studied (Peters, 1959; Viezee andSingh, 1980). It has also been used in studies of the residence timeand deposition of aerosols from the troposphere (Baskaran andShaw, 2001; Liu et al., 2001; McNeary and Baskaran, 2003, 2007;Papastefanou and Ioannidou, 1991, 1996; Rosner et al., 1996).

Deposition of 7Be is generally dependent on the location ofsample collection, particularly regarding the latitude, the localclimate, and the time of season. The precipitation scavengingmechanism of 7Be in air may depend on the precipitationmode, e.g.rain or snow (Hasegawa et al., 2007; Ioannidou and Papastefanou,2006; Kim et al., 2000b). But the predominant process in theentire precipitation phenomenon of 7Be in air is rainout (Ishikawaet al., 1995). A relationship between precipitation and thewashout ratio of 7Be deposition was noted in a high-rainfall area inNew Zealand (Harvey and Matthews, 1989).

Both 7Be and 210Pb have been used to study the environmentalprocesses such as aerosol particle transport and residence times inthe troposphere (Papastefanou and Ioannidou, 1995; Papastefanou,2006), particle deposition velocities (Fogh et al., 1999; Young andSilker, 1980) and particle trapping above ground vegetation(Bondietti et al., 1984). As the sources of 210Pb and 7Be are knownthese radionuclides can also be used as tools for validating atmo-spheric transport models (Koch and Rind, 1998; Koch et al., 1996;Rehfeld and Heimann, 1995).

1.3. Aim of this investigation

We measured the air concentrations of 222Rn (radon) and itslong-lived daughters 210Pb and 210Po during our first polar expe-dition (Ymer-80) during the summer 1980 in the North Atlantic andArctic Ocean north of latitude 75�N, on board the Swedish ice-breaker ‘HMS Ymer’. The recorded average air concentration of

Please cite this article in press as: Persson, B.R.R., Holm, E., 7Be, 210Pb, aEnvironmental Radioactivity (2014), http://dx.doi.org/10.1016/j.jenvrad.2

222Rn was 75 � 21 (SD) mBq/m3 and of 210Pb 0.075 � 0.028 mBq/m3. Themean aerosol residence timewas estimated to be as high as4e7 days in the Arctic air due to low amount of precipitation(Samuelsson et al., 1986). The aerosol residence time of 4e7 dayswould correspond to 210Po/210Pb activity ratio of <0.05.

In the present work we present the results of air concentrationsof 210Pb, 210Po as well as 7Be in surface air measured during suc-ceeding expedition in the Swedish Polar Research program to theAntarctica (1988e1989), the Arctic Ocean (1991) and along thecoastline of Siberia (1994),

2. Material and methods

2.1. Air sampling

During the cruises air filter samples were taken with a so calledAndersen sampler (filter size 0.25 � 0.25 m membrane filter, flowrate 100 m3/h). Air volumes of about 1500 m3 were collected ateach occasion. The sampler had previously taken part in an inter-calibration of samplers (Vintersved, 1994). During the Arctic-91expedition the Andersen sampler was compared with a FOAtransportable reference high volume air sampler (filter size0.56 � 0.56 m microsorban filter, 1100 m3/h). The samplers wereplaced close together on the same deck of the cruise vessel. Theresults for the Anderson sampler based on 7Be were corrected tothat of the FOA sampler. Whenever possible the filters were sent bymail from the ship to the institute for analysis.

2.2. Analysis of the filters

The time between collection and analysis of the filters wasmaximum 2 months. Filters were sent by mail whenever possiblefrom Longyearbyen (Arctic samples) or Montevideo or Marambio(Atlantic and Antarctic samples) whenever possible. Personnelreturning from 1st legs were also involved in this operation.

The filters were measured for 7Be by gamma spectrometry usinga high performance Germanium detector (HpGe Canberra). Afteradding 209Po as radiochemical yield determinant, the samples werewet-ashed by using a mixture of concentrated nitric acid and per-chloric acid. Polonium was spontaneously deposited on nickeldiscs and measured by alpha spectrometry using surface ionimplanted silicon detectors.

Remaining traces of poloniumwere removed by anion exchange.The solutionwas then kept for about 8months, to allow in-growth of210Po from 210Pb to equilibrium. Corrections were done using con-ventional formulae for build-up from210Pb fromsampling to analysis.Decay correction from measurement of Po to plating date was alsodone. All appropriate corrections for radioactive decay were done.

210Bi has a short half life and is in radioactive equilibrium with210Pb. Eventual in situ build up from 210Bi is if any relatively small.The activity of ingrown 210Po was then calculated as describedabove, and finally the activity concentrations of 210Po and 210Pb inair were calculated. 210Pb was analysed after waiting for about 1year for build up after removing of eventual remaining 210Po afterplating. A new 209Po yield determinant was added. A systematicallyerror could occur if some 210Pb is lost at plating of 210Po whichwould give a too high 210Po/210Pb ratio. Several samples of differentmatrixes have been analysed year after plating and have not foundany 210Pb supporting 210Po.

The chemical yield of measurement of 210Pb is the same as for210Po (i.e. 70e80%) since it is based on measurement of 210Po. Thesamples were taken mainly over open water and air has travelledsome time. There is a very small emission of 222Rn over ocean.There might be a different deposition velocity of 210Po compared to210Pb over ice and snow.


Fig. 2. Cruise route in the Arctic Ocean 1991.

B.R.R. Persson, E. Holm / Journal of Environmental Radioactivity xxx (2014) 1e11 3

2.3. Cruise routes and sampling stations

2.3.1. SWEDARP 1988e1989The Swedish Antarctic Research Expedition named “SWEDARP”

was performed during October 1988 through April 1989 with theair sampling device installed on board the ship M/S Stena Arctica.The route of the Swedarp expedition is displayed in Fig. 1.

We started in Gothenburg (67.4�N 12�E) with the first destina-tion Montevideo (34.8�S 56.2�W). From Montevideo we continuedto the Swedish permanent base “Svea” at the North shelf ofAntarctica. After unloading supply and equipment for the conti-nental research group the ship continued to the Argentinean base“Marambio”. The expedition members were allowed to visit thebase with the remains of the stone-hut on “Paulet Island” whereCaptain C.A. Larsen stayed, after his vessel “Antarctic” sank in 1903.

2.3.2. Arctic Ocean 1991The polar expedition “Arctic Ocean” during 1991 surveyed the

Arctic Ocean with the Swedish icebreaker ‘HMS Oden’. The route ofthe Arctic Ocean expedition is displayed in Fig. 2. We started inGothenburg and went directly out in the Arctic Ocean and backagain.

2.3.3. Tundra 1994By participating in the joint Swedish-Russian “Tundra Ecology-

94” expedition 1994 we were given an opportunity to study the airconcentrations of 210Pb and 210Po along a coastline of 3500 km-from the Kola Peninsula 10�E to Kolyuchinskaya Bay 173�E. Thelarge Russian ice-breaking research vessel “R/V Akademik Fedorov”was used as a platform for the expedition. The air sampling devicewas installed on board at Gothenburg and air sampling was per-formed during the route along the Norwegian and North Siberiancoastlines. In Table 1 is given locations of the various places wherewe were transferred the ship to shore with helicopters.

3. Results

3.1. Swedarp 1988e1989

The activity concentrations of 7Be as well as 210Pb, and 210Po inthe surface air as recorded on the routes Gothenburg 57�43’N11�59’E e Montevideo 34�50’S 56�11’W and return. In Table 2 isgiven the results of average activity concentrations of 7Be (mBq/

Fig. 1. Route of the SWEDARP expedition 1988e1989.


m3). 210Pb and 210Po (mBq/m3) in the surface air measured duringvarious intervals of the route Gothenburg 57�43’N 11�59’E e

Montevideo 34�50’S 56�11’W e Antarctica and return.In Table 3 are given the result of average activity concentrations

of 7Be (mBq/m3), 210Pb (mBq/m3), and 210Po (mBq/m3) in the surfaceair on the routes Gothenburg 57�430N 11�590E e Montevideo34�500S 56�110W e Antarctica and return.

The activity concentration of 7Be in the South Atlantic down toAntarctica varied between 1.3 and 1.7 with an average of1.5� 0.8 mBq/m3. At the Equator and up to Gothenburg the averageactivity concentration of 7Be was 4.3 � 0.7 mBq/m3.

The activity concentration of 210Pb in the South Atlantic down toAntarctica during FebruaryeMarch 1989 varied between 11 and58 mBq/m3. At the Equator the average activity concentration of210Pb in November 1988 was about 630 � 170 and in April 1989about 260 � 210 mBq/m3. The average activity concentration of210Pb during the route GothenburgeMontevideo in 1988 was about290� 270 and on the returnMontevideoeGothenburg it was about230 � 140 mBq/m3.

The activity concentration of 210Po in the South Atlantic down toAntarctica during FebruaryeMarch 1989 varied between 6 and14 mBq/m3. At the Equator the average activity concentration in Nov1988 was about 132 � 45, and in April 1989 about 70 � 60 mBq/m3.The average activity concentration of 210Po during the routeGothenburgeMontevideo in 1988 was about 63 � 58, and on thereturn MontevideoeGothenburg it was about 60 � 44 mBq/m3.

3.2. Arctic Ocean 1991eJuly 28>October 04

The activity concentrations of 7Be (mBq/m3), 210Pb (mBq/m3),and 210Po (mBq/m3) as measured during 1991 from July 28 toOctober 4 in the surface air over the Arctic Ocean during 1991 aregiven in Table 4. The ratios of air concentrations of 7Be, 210Pb and210Po in Arctic 1991-07-28 to 1991-10-04 are given in Table 5.

During the cruise in the Arctic Ocean 1991-07-28 to 1991-10-04the average activity air concentrations recorded of 7Be were0.6� 0.4 mBq/m3, 210Pb 46� 34 mBq/m3 and 210Po 37� 23 mBq/m3.

3.3. TUNDRA 1994 e June 08>September 08

In Table 6 is given the activity concentrations of 7Be (mBq/m3),210Pb, and 210Po (mBq/m3) as measured during 1994-June8 < September 8 at the joint Swedish-Russian Tundra Ecology-94


Table 1Expedition route and research sites of the “Tundra Ecology-94” expedition.

Visitingdate 1

On returndate 2

Site no. Name Position

06-04 09-08 Gothenburg 57.43�N 11.98�E06-08[09 09-02 Murmansk 68.57�N 44.10�E06-10 08-31 1(27) Kachkovsky Bay.

Kola Peninsula67.30�N 41.00�E

06-12[13 08-29[30 2(26) North-EasternKanin Peninsula

68.15�N 6.00�E

06-14[15 08-26[28 3(25) Kolguyev Island 69.15�N 50.00�E06-15[16 08-25[26 4(24) Pechora Bay 68.5�N 54.00�E06-17[20 08-22[08-23 5(23) Western Yamal

Peninsula70.45�N 67.00�E

06-21[22 08-20[21 6 (22) Belyi Island.Northern YamalPeninsula

73.00�N 70.00�E

06-22[23 08-18[19 Dickson06-23 7 Arctic Institute

Islands75.00�N. 82.00�E

06-24[26 08-15[17 8(21) North West ofTaymyr Peninsula

76.00�N 94.00�E

06-27[28 08-13[14 9(20) ChelyuskinPeninsula

77.20�N 102.00�E

08-29[30 08-10[11 10(19) North-east ofTaymyr Peninsula

76.00�N 112.00�E

07-03[05 Khatanga rotationpoint 1

74.00�N 110.00�E

07-05[06 11 Olenekskiy Bay 73.15�N 120.00�E08-08[08-08 Tiksi rotation

point 274.00�N 110.00�E

08-03[08-04 12 Yana Delta 71.30�N 136.00�E07-10[11 07-31[08-02 13 New Siberian

Islands75.00�N 140.00�E

07-14[15 14 Lopatka Peninsular,NeW Indigirka

71.45�N 149.00�E

07-17[18 15 North-east ofKolyma Delta

71.45�N 158.00�E

07-20[21 16 Ayon Island 69.50�N 168.00�E07-22[26 17 South-western

Wrangels Island70.50�N 179.00�E

07-25 Point of return 18 KolyuchinskayaBay

67.00�N 173.45�E


expedition. The ratios of average air concentration ratios of 7Be and210Pb measured during 1994eJune 8>September 8 at the jointSwedish-Russian Tundra Ecology-94 expedition are given inTable 7.

During the Swedish-Russian Tundra Ecology-94 expeditionalong the Siberian coastline, the average air concentrations of 7Beand 210Pb measured during MayeJuly were 11 � 3 and

Table 2Average activity concentrations of 7Be (mBq/m3), 210Pb, and 210Po (mBq/m3) in the surfac34�50’S 56�11’W e Antarctica and return.

Time Latitude Longitude Number ofsamples

7Be

mBq/m

N(þ)/S(�) W(�)/E(þ) Ave.

1988 1124>1130 34.5>14 �12.5>�56 61988 1201>1205 9.5 � 11.5 �25 � �56 61988 1124>1212 34 � 35 �12.5>�56 51988 1213>1227 �35>�70 �56>�8.5 151989 0101>0205 �72>�70 �16>�8 151988 1228>89 0205 �70>�70 �10>�8 231989 0211>0318 �64>�60.5 �50>�58 33 1,31989 0319>0324 �56.5>�35 �59>�56 6 3,41989 0206>0324 �70>�35 �13.5>�56 39 1,71989 0401>0407 12.5 � 13 �28.5>�23.5 7 4,31989 0325>0417 �35>N 52 �56>3 24 4,3


2.4 � 0.4 mBq/m3 respectively and during JulyeSeptember theywere 7.2 � 2 and 2.7 � 1.1 mBq/m3 respectively.

4. Discussions

4.1. Beryllium-7 activity concentrations in the Arctic air

The activity concentration of 7Be in air in the Arctic air assummarized in Table 8 varies between 2 and 4.9 mBq/m3 with anaverage of 2.8 � 0.3 mBq/m3 (Aldahan et al., 2001; Baskaran andShaw, 2001; Dibb and Jaffrezo, 1993; Kulan et al., 2006a,b;Paatero and Hatakka, 2000). But the average of 7Be activity-concentration in air over the Arctic Ocean as we recorded wasonly about 0.6 mBq/m3. In contrast the activity concentration of 7Bein air close to the Siberian coast-line as high as 11 mBq/m3 (Perssonand Holm, 2013).

4.2. 210Pb and 210Po activity concentrations in the Arctic air

Observations of the activity concentration of 210Pb in the air overthe Arctic Ocean as summarized in Table 9 vary between 37 and176 mBq/m3 (Dibb and Jaffrezo, 1993; Dibb, 2007; McNeary andBaskaran, 2003; Paatero et al., 2003; Persson and Holm, 2013;Samuelsson et al., 1986). In 1991 we found the average activityconcentration of 210Pb over the Arctic Ocean to be 40� 4 mBq/m3. Inthe air close to landmasses the activity concentration of 210Pb in theair was 269e2712 mBq/m3, with the highest values at the Siberiancoastline (Persson and Holm, 2013).

As seen from Table 9 most observations of the activity concen-tration of 210Po in the Arctic air vary between 23 and 38 mBq/m3

(Baskaran and Shaw, 2001; Persson and Holm, 2013; Samuelssonet al., 1986). A higher value of 100 mBq/m3 was observed in 1996at Alaska USA Poker Flat (Baskaran and Shaw, 2001).

4.3. Beryllium-7 activity concentrations in the Antarctic air

The activity concentrations (mBq/m3) of 7Be in the Antarctic airreported from various authors are displayed in Table 10 (Elsaesseret al., 2011; Persson and Holm, 2013; Sanak et al., 1985). Theaverage activity concentrations of 7Be are 3.3 � 2.0 mBq/m3. Thusthe agreement of the results from the various authors is in rathergood although the results are scattered in time between 1988 and1999. There seems, however to be a group of lower 7Be levels1.43 � 0.19 mBq/m3 around latitudes (65-62�S) (Persson and Holm,2013).

e air on various segments on the route Gothenburg 57�43’N 11�59’E e Montevideo

210Pb 210Po

3 mBq/m3 mBq/m3

SD Min Max Ave. SD Min Max Ave. SD

83 251 163 61 25 47 36 9501 948 626 169 104 218 132 4540 149 288 268 7 61 63 585 126 45 45 3 50 21 174 46 22 9 6 58 9 34 46 24 11 6 58 13 14

0,6 4 56 15 13 2 20 6 40,9 157 566 305 227 24 127 61 581,0 4 566 58 126 2 127 14 270,3 119 570 262 207 33 159 69 601,1 101 570 232 140 4 159 60 44


Table 3Average activity ratios (�SD) of 7Be/210Pb, and 7Be/210Po at various route sections recorded during the Swedarp expedition 1989.

Date Latitude Longitude Activity Ratio Location

1989 7Be/210Pb 7Be/210Po

0211>0318 S64>S60.5 W50>W58 8.7 � 8.4 22.2 � 16.1 Antarctica0319>0324 S56.5>S 35 W59>W56 1.1 � 0.9 5.6 � 5.5 AntarcticaeMontevideo0206>0324 S70>S35 W13.5>W56 2.9 � 6.6 12.0 � 48 South Atlantic0401>0407 N12.5>S13.5 W28.5>W23.5 1.7 � 1.3 6.3 � 4.9 Equator0325>0417 S35>N52 W56>E3 1.9 � 1.2 7.2 � 4.4 Montevideo[Gothenburg

Table 4Air concentrations of 7Be, 210Pb and 210Po in Arctic Ocean during 1991-07-28 to1991-10-04 Pb-21.

Isotope Date Average Standard deviation Standard error

Be-7 910728-0906 0.62 0.52 0.14 mBq/m3

Pb-210 910728-0906 49.2 46.2 12.8 mBq/m3

Po-210 910728-0906 36.8 28.5 7.9 mBq/m3

Be-7 910907-1004 0.51 0.33 0.09 mBq/m3

Pb-210 910907-1004 43.8 21.4 5.7 mBq/m3

Po-210 910907-1004 37.6 17.2 4.6 mBq/m3

Table 5Ratios of air concentrations of 7Be, 210Pb and 210Po in Arctic Ocean 1991-07-28 to1991-10-04 Pb-21.

Isotope ratio Date Average SE

Be-7/A/Pb-210 A 910728-0906 12 4Be-7 A/Po-210 A 910728-0906 17 5Be-7 B/Pb-210 B 910907-1004 12 3Be-7 B/Po-210 B 910907-1004 13 3

Table 6Average air concentrations of 7Be and 210Pb measured during 1994-June8>September 8 at the joint Swedish-Russian Tundra Ecology-94 expedition.

Isotope Date Average SD SE

Latitude 71 4 1 NLongitude 84 47 11 E7Be 1994-0605>0719 11.4 9.0 3.2 mBq/m3

210Pb 1994-0605>0719 2373 1029 364 mBq/m3

7Be 1994-07-19>0908 7.2 5.4 2.0 mBq/m3

210Pb 1994-07-19>0908 2712 2854 1079 mBq/m3

Table 7Ratios of average air concentration ratios of 7Be and 210Pb measured during 1994-June 8>September 8 at the joint Swedish-Russian Tundra Ecology-94 expedition.

Isotope ratio Date Average SE

Latitude 71 1Longitude 84 117Be/210Pb 1994-0605>0719 5 27Be/210Pb 1994-07-19>0908 3 1

Table 8Summary of atmospheric 7Be concentrations in Arctic and sub-Arctic air.

Time Location Lat Long Be-7 SD Reference

Arithm.Mean

Nþ; S� Eþ; W� mBq/m3

910728-0906 Arctic Ocean 82.07 51.00 0.62 0.52 This worka

910907-1004 Arctic Ocean 84.36 �2.32 0.51 0.33 This worka

940605-0908 N Siberiancoast

71 84 11.4 9.0 This worka

2000 Uppsala.Sweden

59.88 17.63 4.7 2.3 Aldahan et al.,2001

1972-1995 Sweden 59.88 17.63 4.8 2.4 Aldahan et al.,2001

1972e2003 Sweden.Kiruna

67.84 20.34 1.9 1.0 Kulan et al.,2006a,b

1972e2003 Sweden.Grindsjön

59.07 17.82 2.3 1.2 Kulan et al.,2006a,b

1972e2003 Sweden.Ljungbyhed

56.08 13.23 2.5 1.3 Kulan et al.,2006a,b

1995e1997 FinlandSodankyla

67.37 26.65 2.5 2.0 Paatero andHatakka, 2000

1996 Alaska USA:Poker Flat

65.13 �147.48 3.0 2.0 Baskaran andShaw, 2001

1996 Alaska USAEagle

65.9 �141.20 2.2 1.0 Baskaran andShaw, 2001

1988e1989 Dye3 65.18 43.82 2.6 1.1 Dibb and Jaffrezo,1993

1988e1990 Barrow 71.30 �156.77 1.9 1.1 Dibb and Jaffrezo,1993

1988e1991 Kap Toban 70.42 �21.97 2.4 1.3 Dibb and Jaffrezo,1993

1988e1992 Nord 81.36 �16.40 2.5 1.4 Dibb and Jaffrezo,1993

1988e1993 Thule 77.50 �69.33 3.7 1.9 Dibb and Jaffrezo,1993

1997e2004 Summit.Greenland

72.575 �27.55 2.0 0.5 Dibb, 2007

a Persson and Holm, 2013.


4.4. 210Pb and 210Po activity concentrations in the Antarctic air

The activity concentrations (mBq/m3) of 210Pb and 210Po in airover Antarctica as reported from various authors are displayed inTable 11 (Elsaesser et al., 2011; Lambert et al., 1990; Persson andHolm, 2013). The average activity concentrations of 210Pb are


27� 10 mBq/m3 omitting the extreme value of 305 mBq/m3 inMarch1989. Thus the results from the various authors are in very goodagreement, despite scattered around in time during 1988e2008.The activity concentrations of 210Po as reported by this work only,with an average of 12 � 7 mBq/m3.

4.5. Results of present work compared with others

4.5.1. 7Be, 210Pb and 210Po activity concentrations in the Arctic airThe activity concentration of 7Be in the Arctic air, as reported by

various authors including the present work, varies between 2 and5 mBq/m3 with an average of 2.8 � 0.3 mBq/m3. We found, how-ever, that the average of 7Be activity concentration in air over theArctic Ocean was as low as 0.6 mBq/m3. This is in contrast to airclose to the Siberian coast-line, where the activity concentration of7Be was as high as 11 mBq/m3 (Persson and Holm, 2013).

In 1991 we found the average activity concentration of 210Pbover the Arctic Ocean to be 40 � 4 mBq/m3 which is somewhat


Table 9Activity concentrations (mBq/m3) of 210Pb and 210Po in Arctic air recorded at different locations.

Time Location Lat Long Pb-210 SD Po-210 SD Reference

Nþ; S� Eþ; W� Average Average

mBq/m3 mBq/m3

910728-0906 Arctic Ocean 91 82.07 51.00 37 8 37 8 This work910907-1004 Arctic Ocean 91 84.36 �2.32 44 6 38 5 This work940605>0703 Siberian Tundra 71 84 2373 364 This work940704>0908 Siberian Tundra 71 84 2712 1079 This work2002 Detroit. USA 42.23 �83.33 1152 818 McNeary and Baskaran, 20031995e1997 Finland Sodankyla 67.37 26.65 160 110 Paatero and Hatakka, 20001996 Alaska USA Poker Flat 65.13 �147.48 922 100 100 52 Baskaran and Shaw, 20011996 Alaska USA Eagle 65.90 �141.20 369 45 23 10 Baskaran and Shaw, 20011988e1989 Dye3 65.18 43.82 176 20 Dibb and Jaffrezo, 19931988e1990 Barrow 71.30 �156.77 433 93 Dibb and Jaffrezo, 19931997e2004 Summit. Greenland 72.58 �27.55 96 17 Dibb, 20072001 Svalbard Ny-Ålesund 78.97 12.05 134 13 Paatero et al., 20031980 Arctic Ocean 75 45 75 28 22.5 8.4 Samuelsson et al., 1986


lower than the values 75e176 mBq/m3 previously reported byothers. In the air close to the Siberian coastline, the activity con-centration of 210Pb in the air is increased to values up to about2500 mBq/m3 (Persson and Holm, 2013). Most observations of theactivity concentration of 210Po in the Arctic air vary between 23 and38 mBq/m3. But a higher value of 100 mBq/m3 was observed in 1996at Alaska (Baskaran and Shaw, 2001).

4.5.2. 210Pb and 210Po activity concentrations in the Atlantic airDuring NovembereDecember 1988 the average activity con-

centrations of 210Pb and 210Po in the North Atlantic 34.5e14�N,12.5e56�W were 160 and 40 mBq/m3 respectively. While aroundthe equator 9.5�Ne11.5�S, 25e56�W the activity concentrations of210Pb and 210Po increased to 630 and 170 mBq/m3 respectively. Inthe South Atlantic 35e70�S, 56e8.5�W the average activity con-centration of 210Pb was 45 mBq/m3 and of 210Po 29 mBq/m3.

During MarcheApril 1989 the average activity concentrations of210Pb and 210Po around the equator 9.5�Ne11.5�S, 25e56�Wdecreased to 260 and 70 mBq/m3 respectively. In the South Atlantic35e70�S, 8.5e56�W the average activity concentrations of 210Pband 210Po were 60 and 14 mBq/m3 respectively.

The average concentration over the whole cruise GothenburgeMontevideoeGothenburg average activity concentrations of210Pb and 210Po was 250 and 60 mBq/m3 respectively.

4.5.3. 7Be, 210Pb and 210Po activity concentrations in the Antarcticair

The average activity concentrations of 7Be in Antarctic as re-ported by various authors including this work are around 3.3 � 2.0(mBq/m3). The agreement of the results from the various authors is

Table 10Activity concentrations (mBq/m3) of 7Be in Antarctic air recorded at different locations.

Time Location Lat Lo

Nþ; S� Eþ

1989 0206>890324 South Atlantic �61.47 �51989 0211>890318 Antarctica �63.52 �51989 0319>890324 AntarcticaeMontevideo �44.33 �51983e2008 Neumayer �70.651970e1999 South Pole �90.001987e1993 Mawson �67.60 61990e#e1999 Palmer �64.77 61990e1993 Marsh �62.18 51978e1981 Dumont d’Urville �66.67 14


in rather good agreement, although scattered around in time(1988e1999).

In the Antarctic air the average of all reported activity concen-trations of 210Pb is 27 � 10 mBq/m3, with the extreme value of305 mBq/m3 inMarch 1989 omitted. The agreement with the resultsfrom the various authors is in very good agreement despite scat-tered around in time (1988e2008). The average activityconcentration of 210Po is 12 � 7 mBq/m3 as reported only by thepresent study (Persson and Holm, 2013).

4.5.4. Global distribution of 7BeThe Longitudinal distribution of all reported all concentrations

of 7Be (mBq/m3) is displayed in Fig. 3 and the corresponding lat-itudinal distribution is displayed in Fig. 4.

4.5.5. Global distribution of 210PbDeposition rates are usually described by the deposition veloc-

ities Vd and Vdd (in mm/s) for total (wet and dry) and dry depositionvelocities, respectively (Papastefanou and Ioannidou, 1991; Toddet al., 1989; Turekian et al., 1983). The total flux of 210Pb to theearth’s surface F (Bq/m2/a) is given by the relation:

F ¼ Cair$Vd

�3:17$10�8

�

where

F deposition flux (Bq/m2/a)Vd deposition velocity for total (wet and dry) (mm/s),Cair is the surface level activity concentration (Bq/m3) of 210Pb atthe sampling site.

ng Be-7 Be-7 Reference

; W� Arithm. mean SD

mBq/m3 mBq/m3

4.60 1.7 1 This work8.64 1.3 0.6 This work8.25 3.4 0.9 This work8.25 4.30 1.2 Elsaesser et al., 20110.00 4.20 2.1 Elsaesser et al., 20112.55 5.40 2.1 Elsaesser et al., 20114.07 1.30 0.5 Elsaesser et al., 20118.98 1.40 0.5 Elsaesser et al., 20110.02 6.80 1.4 Sanak et al., 1985


Table 11Activity concentrations (mBq/m3) of 210Pb in Antarctic air recorded at different locations.

Time Location Lat Long Pb-210 SD Po-210 SD References

Nþ; S- Eþ; W- Average conc. Average conc.

mBq/m3 mBq/m3

1988 Dec MontevideoeAntarctica �53.00 �29.80 45 45 21 17 This work1988e1989 Antarctica �72.43 �25.74 24 11 13 14 This work1989 Jan Antarctica �73.00 �31.27 22 9 9 3 This work1989e1989 Antarctica �63.52 �58.64 15 13 6 4 This work1989 March AntarcticaeMontevideo �44.33 �58.25 305 227 61 58 This work1960e1986 Dumont. Antarctica �66.67 140.02 30 10 Lambert et al., 19901976e1999 South Pole. Antarctica �90.00 0.00 36 20 Elsaesser et al., 20111983e2008 Neumayer. Antarctica �70.65 8.25 34 8 Elsaesser et al., 20111987e1993 Mawson. Antarctica �67.60 62.55 30 10 Elsaesser et al., 20111990e1999 Palmer. Antarctica �64.77 64.07 15 7 Elsaesser et al., 20111990e1999 Marsh. Attica �62.18 58.98 17 7 Elsaesser et al., 2011


By using the value 12.1 � 4.5 mm/s, for the total depositionvelocity, in this relation we converted our recorded values of airactivity concentrations to deposition flux values (Bq/m2/a) (Likukuand Branford, 2011). The latitudinal distribution the 210Pb deposi-tion flux of our results thus obtained together with other reportedvalues are given in Table 12 and displayed in Fig. 5 the datacompiled by Baskaran (2011).

The fitted curve of the data in Table 11 and displayed in Fig. 5 isfitted by the equation:

10logðFÞ[2:14þ 6:5$10�3$XL1:61$10�4$X2L1:26$10�7$X3L7:4$10�9$X4

The fitting equation of the data compiled in Table 12 agreesextremely well with the fitting equation of the data compiled to thevalues given by Baskaran (2011).

Fig. 3. Longitudinal distribution of all reported air concentrations of 7Be (mBq/m3).

10logðlatÞ[2:16þ 9:45$10�3$XL7:45$10�5$X2L6:36$10�7$X3L1


The average value of the 210Pb surface air concentration between60�S and 90�S is 28 � 13 mBq/m3 which is in good agreement withthe value of 30 estimated by a global atmospheric transport model(Balkanski et al., 1993).

4.5.6. Global distribution of 210PoThe 210Po/210Pb-activity ratio recorded in the surface air during

all our expeditions is displayed in Fig. 6a and b.

The 210Po/210Pb-activity ratio recorded in the surface air betweenthe latitudes 55�N and 35�S was quite constant with an average of0.25 � 0.15 SD (32 samples). This value recorded in the surface air

Fig. 4. Latitudinal distribution of all reported air concentrations of 7Be (mBq/m3).

:81$10�8$X4


Table 12Compilation of our and published data of 210Pb surface air concentration and estimated average total deposition by applying 210Pb e Total deposition velocity value of 12 mm/sin the equation above.

Location Lat Long Pb-210 SD Pb-210 SD Reference

Nþ; S� Eþ; W� Ave. conc. Ave. dep.

mBq/m3 Bq/m2/a

Arctic Ocean 92 84.36 �2.32 44 6 17 2 This workArctic Ocean 91 82.07 51.00 37 8 14 3 This workEdinburgh, UK 55.95 �3.22 210 10 79 4 Likuku and Branford, 2011England, Chilton 51.5 �1.65 204 98 77 37 Daish et al., 2005Neuherberg, Germany 48.22 11.60 470 140 178 53 Winkler et al., 1998Neuherberg, Germany 48.22 11.60 570 170 216 64 Winkler and Rosner, 2000Puy de Dôme, France 45.77 2.97 850 90 322 34 Bourcier et al., 2011Opme France 45.72 3.07 730 220 276 83 Bourcier et al., 2011Monaco 45.52 7.51 1130 440 428 167 Pham et al., 2011Belgrade, Serbia 44.52 20.32 480 300 182 114 Todorovic et al., 2010Detriot, USA 42.23 �83.33 1152 818 436 310 McNeary and Baskaran, 2003Barcelona, Spain 41.35 2.17 487 34 184 13 Pham et al., 2011Japan (Rokkasho) 40.95 141.35 1010 830 382 314 Akata et al., 2008Spain, Helva 37 �7 591 103 224 39 Lozano et al., 2011Malaga, Spain 36.72 �4.47 580 210 219 79 Duenas et al., 2009Spain, Malaga 36.72 �4.47 540 30 204 11 Duenas et al., 2005Spain, Malaga 36.72 �4.47 580 210 219 79 Duenas et al., 2009Islamabad 33.38 73.1 284 150 107 57 Ali et al., 2011North Atlantic 24.08 �17.17 163 61 62 23 This workIndia, Bay of Bengal 21 �64 960 200 363 76 Rengarajan and Sarin, 2004Montevideo[Gbg. 7.00 �25.02 232 140 88 53 This workEquator 0.29 �26.00 262 207 99 78 This workEquator �0.83 �29.42 626 169 237 64 This workGbg.eMontevideo 25.75 �44.67 288 268 109 101 This workAntarcticaeMontevideo 44.33 �58.25 305 227 115 86 This workMontevideoeAntarctica 53.00 �29.80 45 45 17 17 This workSouth Atlantic 61.47 �54.60 58 126 22 48 This workMarsh, Attica 62.18 58.98 17 7 6 3 Elsaesser et al., 2011Antarctica 63.52 �58.64 15 13 6 5 This workPalmer, Antarctica 64.77 64.07 15 7 6 3 Elsaesser et al., 2011Dumont, Antarctica 66.67 140.02 30 10 11 4 Lambert et al., 1990Mason, Antarctica 67.60 62.55 30 10 11 4 Elsaesser et al., 2011Niemeyer, Antarctica 70.65 8.25 34 8 13 3 Elsaesser et al., 2011Antarctica 72.43 �25.74 24 11 9 4 This workAntarctica 73.00 �31.27 22 9 8 3 This work


over the Atlantic Ocean between the latitudes 55�N and 35�S ishigher than corresponding values reported from continental air(Baskaran, 2011; Yi et al., 2007). The residence time of ambientaerosols in 30 samples of ocean air between the latitudes 55�N and35�S was estimated to 60 � 4(SE) d which is much higher than in

Fig. 5. Latitudinal distribution of all reported average values of deposition flux (F) of210Pb (Bq/m2/a). The square dots are the data given in Table 12 and the open circles thedata compilation of Baskaran (2011).


continental air (Rastogi and Sarin, 2013). High 10Po/210Pb-activityratio over ocean has also been found from measurements in theChesapeake Bay atmosphere, where 210Po/210Pb-activity ratioincreased with wind speed (Kim et al., 2000a). According to theirresults, a 210Po/210Pb-activity ratio value of 0.25 corresponds to amaximum wind speed of 8 m/s.

But the activity ratio starts to increase towards the poles wherethe 210Po/210Pb-activity ratio reached a value of about 0.9e1.1. Ac-cording to Kim et al. (2000a,b) the 210Po/210Pb-activity ratioreached a value of 0.8 at a wind speed of 10 m/s, which they explainby sea-air exchange of volatile Po along with other bio volatilespecies in the surface ocean during high wind speeds (Kim et al.,2000a).

The Latitudinal distribution of 210Po from Arctic to Antarcticadisplayed in Fig. 7 is achieved by convolution of the fitting equa-tions of Figs. 5 and 6.

5. Conclusion

In the present study we have investigated the activity concen-trations of 210Pb and 210Po as well as 7Be in surface air duringsucceeding expedition in the Swedish Polar Research program ofthe North and South Atlantic (Antarctica) (1988e1989), the ArcticOcean (1991), and along the coastline of Siberia (1994).

At the cruise in the Arctic Ocean during 1991-07-28 to 1991-10-04 the average air concentrations of 7Be was 0.6 � 0.4 mBq/m3.The activity concentration of 7Be in the Arctic air, as reported by


Fig. 6. a. The 210Po/210Pb-activity ratio recorded in the surface air of all individual samples during our expeditions. b. The average over latitude intervals of 10� of 210Po/210Pb-activityratio recorded in the surface air of all individual samples during our expeditions. The data was fitted to a 2nd degree polynomial to be used for converting the 210Pb activitydistribution of Fig. 5 the 210Po distribution of Fig. 7.


various authors varies between 2 and 5 mBq/m3 with an average of2.8 � 0.3 mBq/m3 which is slightly higher than our recorded valuesin the Arctic Ocean. But during the Swedish-Russian Tundra

10logðFÞ[2:14þ 6:5$10�3$XL1:61$10�4$X2L1:26$10�7$X3L7:4$10�9$X4

Fig. 7. Latitudinal distribution of air concentrations of 210Po (mBq/m3). Estimated from:[Latitudinal distribution of 210Pb] � [210Po/210Pb-activity ratio].

Ecology-94 expeditionwe recorded close to the Siberian coast-line,an activity concentration of 7Be as high as 11 mBq/m3.

At the cruise in 1991 we found the average activity concentra-tion of 210Pb over the Arctic Ocean to be 40 � 4 mBq/m3 which issomewhat lower than the values 75e176 mBq/m3 previously re-ported by others. But during the Swedish-Russian Tundra Ecology-94 expedition we recorded an activity concentration in air close tothe Siberian coastline as high as 2500 mBq/m3.

We found that the average activity concentration of 210Po in theArctic Ocean air was 38 � 10 mBq/m3 which agrees well with 210Poactivity concentration between 23 and 38 mBq/m3 reported byothers.

The activity concentration of 7Be in the South Atlantic during thecruise down to Antarctica varied between 1.3 and 1.7 with anaverage of 1.5 � 0.8 mBq/m3.

The 210Pb activity concentration in the South Atlantic down toAntarctica varied between 6 and 14 mBq/m3. At the Equator theactivity concentration recorded in November 1988 was 630 mBq/m3

and in April 1989 it was 260 mBq/m3. The average activity con-centration of 210Pb during the route GothenburgeMontevideo in1988 was 290 and at the return MontevideoeGothenburg it was230 mBq/m3.

The activity concentration of 210Po in the South Atlanticdown to Antarctica varied between 15 and 58 mBq/m3. At theEquator the activity concentration in November 1988 was 170and in April 1989 70 mBq/m3. The average activity concentra-tion of 210Po during the route GothenburgeMontevideo in 1988was 63 and on the return MontevideoeGothenburg it was60 mBq/m3.

The average of the activity concentration of 210Pb in Antarctic airwas 27 � 10 mBq/m3, and of 210Po it was 12 � 7 mBq/m3. Theagreement with the results from the various authors is in very good,despite scattered around in time (1988e2008). 210Po was reportedonly by the present study, with the average activity concentrationof 12 � 7 mBq/m3.


The latitudinal distribution of all values of 210Pb deposition flux(F Bq/m2/a) appears as a rather smooth log-linear plot which couldbe fitted to the equation:

where X is the Latitude in degrees.By multiplying the Latitudinal distribution of the 210Po/210Pb-

activity ratio recorded in the surface during all our expeditionswiththe 210Pb deposition flux, also the Latitudinal distribution of 210Pofrom Arctic to Antarctica is achieved.

The 210Po/210Pb-activity ratio recorded in the surface air be-tween the latitudes 55�N and 35�S was quite constant 0.25 � 0.15SD (32 samples). The ratio started to increase towards the poleswhere the ratio reached a value of about 0.9e1.1. This steady in-crease of the ratio from lower latitudes to the poles, however, is notpreviously discovered and needs further research to explain. It mayhave a major implication to future polar atmospheric research.



Acknowledgements

Wewish to thank Kjell-Åke Carlsson for his skilful managementof the logistics before and during the expeditions and GertieSvensson for her excellent laboratory work. We also want to thankThe Swedish Polar Institute for supporting our participation in theexpeditions. Also the support of The Royal Physiographic Society inLund is greatly acknowledged.

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7Be, 210Pb, and 210Po in the surface air from the Arctic to Antarctica