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Supplementary Information New constraints on elemental and Pb and Nd isotope compositions of South American and Southern African aerosol sources to the South Atlantic Ocean R. Khondoker a , D. Weiss a, * , T. van de Flierdt a , M. Rehkämper a , K. Kreissig a , B. J. Coles a , S. Strekopytov b , E. Humphreys-Williams b , D. Shoufei a,c , A. Bory d , V. Bout-Roumazeilles d , P. Smichowski e , P. Cid-Agüero f , M. Babinski g , R. Losno h , F. Monna i a* Dept. of Earth Science & Engineering, Imperial College London, SW7 2AZ , UK b Natural History Museum, London, SW7 5BD, UK c CRPG, UMR-CNRS 7358, Vandœuvre, Villeneuve d’Ascq Cedex, France d University of Lille, CNRS, University of Littoral Côte d’Opale, UMR 8187, LOG, Laboratoire d’Orceanologie et de Géosciences, F 59000 Lille, France e National Atomic Energy Commission, Av. Gral Paz 1499, Buenos Aires, Argentina f University of Magallanes, Avda. Bulnes, 01855, Punta Arenas, Chile

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Supplementary Information

New constraints on elemental and Pb and Nd isotope compositions of South American and Southern African aerosol sources

to the South Atlantic Ocean

R. Khondokera, D. Weissa, *, T. van de Flierdta, M. Rehkämpera, K. Kreissiga, B. J. Colesa, S. Strekopytovb, E. Humphreys-Williamsb, D. Shoufeia,c, A. Boryd, V. Bout-Roumazeillesd, P. Smichowskie, P. Cid-Agüerof, M. Babinskig, R. Losnoh, F. Monnai

a* Dept. of Earth Science & Engineering, Imperial College London, SW7 2AZ , UK

b Natural History Museum, London, SW7 5BD, UK

c CRPG, UMR-CNRS 7358, Vandœuvre, Villeneuve d’Ascq Cedex, France

dUniversity of Lille, CNRS, University of Littoral Côte d’Opale, UMR 8187, LOG, Laboratoire d’Orceanologie et de Géosciences, F 59000 Lille, France

e National Atomic Energy Commission, Av. Gral Paz 1499, Buenos Aires, Argentina

f University of Magallanes, Avda. Bulnes, 01855, Punta Arenas, Chile

g Geochronological Research Centre, University of São Paulo, São Paulo, Brazil

h LISA Faculty of Science, University of Paris, Batiment P4 393, Paris, France

I Univerisity of Bourgogne, Batiment Gabriel, Dijon, France

*[email protected]

Table S1. Limits of quantitation (LOQ) relevant for the sample solution aliquots analysed by ICP-AES and ICP-MS

Element

LOQ

ICP-AES, ppm

Al

0.1

Fe

0.1

K

0.01

Mg

0.01

Mn

0.02

Na

0.5

Cu

0.05

Pb

0.05

Cd

0.05

Zn

0.02

Cr

0.05

Ni

0.02

Co

0.02

V

0.05

ICP-MS, ppb

La

0.01

Ce

0.03

Pr

0.003

Nd

0.007

Sm

0.002

Eu

0.002

Gd

0.002

Tb

0.002

Dy

0.002

Ho

0.002

Er

0.002

Tm

0.001

Yb

0.002

Lu

0.002

Sc

0.03

Th

0.06

Y

0.005

Analyses of blank samples that were prepared and handled in the same manner as sample solutions consistently yielded concentrations below the LOQ values for all elements.

Table S2. Major element concentrations of samples from South America and Southern Africa, in % (w/w)

Sample ID

Sample Location

Al2O3

CaO

Fe2O3

K2O

MgO

MnO

Na2O

South America

Rural – Topsoil, Bed sediment (bulk)

4

Bahia San Sebastian, Southern Patagonia

4.66

26.8

1.93

0.878

3.76

0.112

1.51

5

Bahia San Sebastian, Southern Patagonia

11.6

1.80

4.41

1.92

2.76

0.115

3.31

8

Bahia San Sebastian, Southern Patagonia

12.8

1.72

5.63

2.23

2.49

0.127

3.46

9

Bahia San Sebastian, Southern Patagonia

12.3

2.31

5.17

2.15

2.49

0.139

3.73

10

Bahia San Sebastian, Southern Patagonia

11.5

1.72

5.21

2.02

2.22

0.126

3.05

11

Bahia San Sebastian, Southern Patagonia

11.3

2.14

4.95

2.00

2.81

0.113

2.93

12

Bahia San Sebastian, Southern Patagonia

11.8

1.85

4.55

1.78

1.68

0.0955

3.12

19

Rio Gallegos, Southern Patagonia

13.2

1.96

5.22

1.43

1.25

0.0482

2.28

21

Rio Gallegos, Southern Patagonia

12.9

3.90

5.55

1.17

1.97

0.131

2.71

35

Rio Santa Cruz, Southern Patagonia

14.1

3.31

4.70

1.65

1.65

0.114

3.02

40

Punta Arenas, Southern Patagonia

14.5

3.84

4.96

0.883

2.85

0.0811

2.43

42

Punta Arenas, Southern Patagonia

15.8

1.16

6.01

0.861

1.27

0.0476

1.39

1

Rio Grande, Southern Patagonia

13.0

2.22

4.93

1.73

1.64

0.0835

2.75

2

Rio Grande, Southern Patagonia

13.4

2.47

5.08

1.89

1.84

0.0675

2.83

13

Rio Grande, Southern Patagonia

11.9

1.52

4.71

1.76

1.47

0.0489

2.57

15

Rio Grande, Southern Patagonia

12.5

2.80

3.93

1.61

1.77

0.0775

4.64

17

Rio Grande, Southern Patagonia

10.6

2.90

3.75

1.22

1.52

0.104

4.17

24

Rio Grande, Southern Patagonia

11.9

2.58

3.79

1.65

1.36

0.0791

3.49

27

Bahia Grande, Southern Patagonia

9.68

2.54

3.01

1.13

1.26

0.0724

2.55

28

Bahia Grande, Southern Patagonia

12.0

3.01

4.51

1.65

2.05

0.101

2.83

30

Rio Santa Cruz, El Calafate, Southern Patagonia

13.0

2.20

4.20

1.61

1.17

0.0461

2.43

32

Rio Santa Cruz, El Calafate, Southern Patagonia

7.32

1.38

2.34

1.00

0.623

0.0298

1.57

33

Rio Santa Cruz, El Calafate, Southern Patagonia

11.8

2.25

4.16

1.72

1.36

0.0645

2.84

38

Argentino Lake, El Calafate, Southern Patagonia

11.6

2.52

4.73

1.37

1.35

0.0871

1.82

Volcanic – Volcanic clasts and tephra (bulk)

CH

Chaiten Volcano, Southern Volcanic Zone

13.5

1.64

1.46

3.07

0.324

0.0563

4.05

PU1

Puyehue Volcano, Southern Volcanic Zone

13.8

2.03

4.42

2.83

0.620

0.107

5.99

PU2

Puyehue Volcano, Southern Volcanic Zone

13.3

1.99

4.15

2.82

0.592

0.0981

5.66

PU3

Puyehue Volcano, lakeside near La Angostura

11.9

1.91

2.75

2.81

0.475

0.0709

4.54

CO

Cotopaxi Volcano, Northern Volcanic Zone

18.2

7.00

8.64

1.52

5.116

0.125

4.63

Table S2. (continued.)

Sample ID

Sample Location

Al2O3

CaO

Fe2O3

K2O

MgO

MnO

Na2O

Urban – Road dusts (50-100μm), Aerosols (<10μm)

3C

Urban Area, Buenos Aires

11.3

3.28

4.10

2.17

1.16

0.0727

2.37

9C

Urban Area, Buenos Aires

10.9

4.74

5.93

2.10

1.39

0.0939

2.32

110C

Urban Area, Buenos Aires

10.2

4.51

5.97

1.86

1.10

0.0864

2.15

112C

Urban Area, Buenos Aires

9.47

4.79

6.01

1.99

1.18

0.0916

1.96

3D

Urban Area, Buenos Aires

9.95

3.23

4.13

2.28

1.20

0.0659

2.02

9D

Urban Area, Buenos Aires

9.66

4.41

4.84

2.17

1.28

0.0774

2.05

110D

Urban Area, Buenos Aires

8.53

4.16

6.04

1.75

1.01

0.0852

1.79

112D

Urban Area, Buenos Aires

10.11

4.63

5.42

1.89

1.13

0.0840

2.09

648

Urban Area, São Paulo

0.543

0.0276

0.658

0.276

0.116

0.0184

0.526

649

Urban Area, São Paulo

0.219

0.157

0.263

0.0103

0.173

650

Urban Area, São Paulo

0.441

0.0204

0.483

0.214

0.116

0.0142

0.736

Southern Africa

Rural – Lichen

PILA

Rural Area, Johannesburg

0.530

7.21

0.329

0.366

0.164

0.0153

0.0187

Urban – Lichen

RIV

Urban Area, Johannesburg

1.08

0.600

0.526

0.759

0.173

0.0130

0.0396

DEL

Urban Area, Johannesburg

1.34

2.98

0.706

0.851

0.206

0.0185

0.0392

CMG

Urban Area, Johannesburg

1.09

0.642

0.627

0.760

0.130

0.0128

0.0181

EMER

Urban Area, Johannesburg

1.61

2.95

0.803

0.577

0.197

0.0174

0.0329

HUDD

Urban Area, Johannesburg

1.16

0.212

0.634

0.667

0.143

0.0158

0.0307

BOT2

Urban Area, Johannesburg

1.05

0.129

0.594

0.786

0.153

0.0105

0.0325

Mine – Tree bark

DRD-TB

Mine Dump Site, Johannesburg

0.312

2.44

0.209

0.0657

0.0769

0.110

0.0266

Table S2. (continued.)

Sample ID

Sample Location

Al2O3

CaO

Fe2O3

K2O

MgO

MnO

Na2O

South America – rural and volcanic sediment, <5 μm

4

Bahia San Sebastian, Southern Patagonia

3.55

n.d.

1.93

0.614

4.30

0.142

0.660

32

Rio Santa Cruz, El Calafate, Southern Patagonia

22.5

1.41

7.55

2.10

1.57

0.0923

0.950

42

Punta Arenas, Southern Patagonia

22.9

0.15

9.07

0.823

1.30

0.0533

0.475

CH

Chaiten Volcano, Southern Volcanic Zone

14.4

1.47

1.68

3.72

0.445

0.063

4.31

PU2

Puyehue Volcano, Southern Volcanic Zone

14.1

1.76

3.76

3.46

0.466

0.101

5.27

Reference Material

USGS G-2

This study (n=12)

13.7

1.88

2.55

4.41

0.719

0.0310

3.86

RSD (%)

3.1

4.9

1.2

3.7

4.2

4.7

4.3

USGS G-2

Reference values

15.39

1.96

2.66

4.48

0.75

0.03

4.08

RSD (%)

1.9

4.1

6.4

2.9

4.0

33

3.2

The reference values for the USGS G-2 Granite reference material are from Gladney et al. (1992). The precision of our G-2 data is 1x relative standard deviation (RSD) calculated from the results of multiple individual analyses (n = 12).

n.d. = not determined.

Table S3. Rare earth element, Cu, Pb, Cd, Zn, Cr, Ni, Co, Y, Th, V, and Sc concentrations for samples from South America and Southern Africa (μg g-1)

Sample ID

Sample Location

La

Ce

Pr

Nd

Sm

Eu

Gd

Tb

Dy

Ho

Er

Tm

Yb

Lu

South America

Rural – Topsoil, Bed sediment (bulk)

4

Bahia San Sebastian, Southern Patagonia

7.72

17.8

2.00

8.01

1.66

0.427

1.58

0.248

1.52

0.311

0.898

0.137

0.864

0.133

5

Bahia San Sebastian, Southern Patagonia

20.1

45.2

5.21

21.0

4.52

1.06

4.14

0.653

3.92

0.814

2.29

0.338

2.14

0.329

8

Bahia San Sebastian, Southern Patagonia

22.2

49.9

5.72

23.0

4.96

1.13

4.56

0.715

4.37

0.881

2.59

0.383

2.48

0.374

9

Bahia San Sebastian, Southern Patagonia

21.5

48.3

5.58

22.4

4.74

1.14

4.43

0.705

4.32

0.874

2.54

0.378

2.41

0.368

10

Bahia San Sebastian, Southern Patagonia

21.0

47.0

5.36

21.6

4.55

1.06

4.29

0.669

4.10

0.826

2.34

0.360

2.29

0.356

11

Bahia San Sebastian, Southern Patagonia

20.7

46.5

5.35

21.6

4.60

1.07

4.26

0.666

4.05

0.820

2.38

0.358

2.30

0.350

12

Bahia San Sebastian, Southern Patagonia

21.9

49.1

5.63

22.5

4.86

1.13

4.37

0.689

4.16

0.839

2.43

0.359

2.31

0.353

19

Rio Gallegos, Southern Patagonia

13.3

27.3

2.84

10.5

2.07

0.635

1.66

0.269

1.68

0.357

1.11

0.178

1.21

0.196

21

Rio Gallegos, Southern Patagonia

18.6

40.4

4.62

18.5

3.84

1.09

3.46

0.530

3.18

0.642

1.82

0.275

1.77

0.267

35

Rio Santa Cruz, Southern Patagonia

19.4

43.3

4.81

19.3

4.07

1.10

3.99

0.627

3.90

0.809

2.34

0.359

2.35

0.366

40

Punta Arenas, Southern Patagonia

14.0

27.9

2.97

11.5

2.10

0.794

1.80

0.264

1.56

0.307

0.837

0.125

0.783

0.117

42

Punta Arenas, Southern Patagonia

7.72

16.7

1.87

7.49

1.59

0.398

1.44

0.239

1.51

0.322

0.943

0.153

1.03

0.162

1

Rio Grande, Southern Patagonia

20.1

44.7

5.20

21.0

4.48

1.10

4.21

0.663

4.08

0.824

2.42

0.359

2.29

0.349

2

Rio Grande, Southern Patagonia

20.9

46.3

5.37

21.6

4.64

1.10

4.42

0.700

4.30

0.876

2.52

0.380

2.46

0.376

13

Rio Grande, Southern Patagonia

22.0

47.8

5.67

22.9

4.87

1.14

4.52

0.699

4.27

0.859

2.51

0.374

2.41

0.375

15

Rio Grande, Southern Patagonia

20.0

44.2

5.15

20.8

4.36

1.10

4.18

0.656

3.98

0.810

2.29

0.347

2.22

0.338

17

Rio Grande, Southern Patagonia

20.3

45.5

5.36

21.7

4.53

1.07

4.32

0.675

4.05

0.814

2.28

0.348

2.17

0.323

24

Rio Grande, Southern Patagonia

17.5

37.9

4.40

17.7

3.68

0.991

3.50

0.543

3.29

0.672

1.94

0.287

1.86

0.285

27

Bahia Grande, Southern Patagonia

17.9

34.9

3.77

14.1

2.68

0.809

2.52

0.417

2.76

0.565

1.71

0.256

1.66

0.250

28

Bahia Grande, Southern Patagonia

17.0

36.6

4.17

16.6

3.56

0.930

3.30

0.519

3.17

0.649

1.91

0.286

1.83

0.293

Table S3. (continued.)

Sample ID

Sample Location

La

Ce

Pr

Nd

Sm

Eu

Gd

Tb

Dy

Ho

Er

Tm

Yb

Lu

30

Rio Santa Cruz, El Calafate, Southern Patagonia

25.6

53.5

6.42

25.4

5.21

1.29

4.67

0.722

4.33

0.873

2.58

0.382

2.44

0.375

32

Rio Santa Cruz, El Calafate, Southern Patagonia

21.9

44.3

5.58

22.4

4.56

1.26

4.52

0.704

4.29

0.867

2.45

0.371

2.38

0.363

33

Rio Santa Cruz, El Calafate, Southern Patagonia

17.8

37.9

4.47

18.0

3.76

0.948

3.57

0.564

3.43

0.697

1.99

0.302

1.95

0.297

38

Argentino Lake, El Calafate, Southern Patagonia

23.0

49.0

5.70

22.5

4.47

1.05

3.95

0.594

3.46

0.693

1.93

0.291

1.86

0.287

Volcanic – Volcanic clasts and tephra (bulk)

CH

Chaiten Volcano, Southern Volcanic Zone

37.2

70.6

7.15

23.1

3.86

0.755

3.27

0.506

2.78

0.573

1.80

0.278

1.99

0.310

PU1

Puyehue Volcano, Southern Volcanic Zone

30.8

69.0

8.66

37.0

8.41

1.61

8.45

1.32

8.89

1.80

5.83

0.833

5.88

0.881

PU2

Puyehue Volcano, Southern Volcanic Zone

30.2

66.9

8.46

36.1

8.27

1.66

8.38

1.30

8.73

1.76

5.75

0.819

5.73

0.869

PU3

Puyehue Volcano, lakeside near La Angostura

24.9

52.8

6.75

29.2

6.77

1.36

7.07

1.09

7.37

1.48

4.79

0.689

4.93

0.739

CO

Cotopaxi Volcano, Northern Volcanic Zone

14.6

27.9

3.52

15.2

3.25

0.961

3.04

0.416

2.54

0.472

1.36

0.190

1.26

0.196

Urban – Road dusts (50-100μm)

3C

Urban Area, Buenos Aires

34.1

64.1

7.74

28.7

5.10

1.10

4.18

0.625

3.73

0.731

2.15

0.331

2.13

0.319

9C

Urban Area, Buenos Aires

45.8

95.1

10.6

40.3

7.36

1.33

5.61

0.794

4.56

0.868

2.49

0.368

2.44

0.381

110C

Urban Area, Buenos Aires

39.2

77.8

8.76

33.8

6.03

1.18

4.71

0.687

3.96

0.787

2.26

0.341

2.34

0.366

112C

Urban Area, Buenos Aires

52.8

106

11.9

43.7

7.15

1.15

5.17

0.735

3.86

0.713

1.91

0.285

1.85

0.279

3D

Urban Area, Buenos Aires

45.9

106

10.1

37.9

6.12

1.16

4.29

0.602

3.42

0.651

1.88

0.280

1.78

0.279

9D

Urban Area, Buenos Aires

42.2

90.1

10.3

39.0

6.49

1.14

4.58

0.608

3.39

0.621

1.77

0.269

1.73

0.266

110D

Urban Area, Buenos Aires

47.9

91.5

10.8

39.6

6.47

1.02

4.31

0.586

3.27

0.597

1.70

0.247

1.64

0.240

112D

Urban Area, Buenos Aires

39.5

81.4

8.87

33.3

5.80

1.11

4.56

0.637

3.68

0.716

2.07

0.301

1.93

0.295

Table S3. (continued.)

Sample ID

Sample Location

La

Ce

Pr

Nd

Sm

Eu

Gd

Tb

Dy

Ho

Er

Tm

Yb

Lu

Urban – Aerosols (<10μm)

648

Urban Area, São Paulo

5.00

6.42

0.572

1.94

0.299

0.0648

0.209

0.0272

0.130

0.0214

0.0676

0.00727

0.0528

0.00593

649

Urban Area, São Paulo

4.13

4.88

0.518

1.31

650

Urban Area, São Paulo

9.95

9.53

0.871

2.62

0.399

0.100

0.286

0.0385

0.219

0.0360

0.0893

0.0113

0.0890

0.0127

Southern Africa

Rural – Lichen

PILA

Rural Area, Johannesburg

5.56

10.6

0.929

3.13

0.492

0.122

0.413

0.0608

0.355

0.0690

0.191

0.0280

0.177

0.0270

Urban – Lichen

RIV

Urban Area, Johannesburg

3.41

7.34

0.755

2.69

0.509

0.0961

0.453

0.0733

0.467

0.0907

0.260

0.0401

0.261

0.0425

DEL

Urban Area, Johannesburg

5.55

12.0

1.19

4.31

0.809

0.153

0.705

0.111

0.689

0.139

0.385

0.0599

0.391

0.0615

CMG

Urban Area, Johannesburg

3.85

8.32

0.868

3.19

0.605

0.119

0.546

0.0865

0.543

0.104

0.293

0.0434

0.276

0.0438

EMER

Urban Area, Johannesburg

4.66

8.91

1.05

3.85

0.703

0.158

0.658

0.105

0.601

0.123

0.342

0.0555

0.337

0.0463

HUDD

Urban Area, Johannesburg

3.70

7.80

0.869

3.25

0.617

0.116

0.564

0.0918

0.539

0.113

0.342

0.0512

0.328

0.0481

BOT2

Urban Area, Johannesburg

3.51

7.12

0.748

2.82

0.555

0.103

0.457

0.0717

0.451

0.0872

0.244

0.0391

0.242

0.0389

Mine – Tree bark

DRD-TB

Mine Dump Site, Johannesburg

2.68

4.04

0.477

1.68

0.275

0.0624

0.245

0.0364

0.203

0.0399

0.105

0.0160

0.0985

0.0146

Table S3. (continued.)

Sample ID

Sample Location

La

Ce

Pr

Nd

Sm

Eu

Gd

Tb

Dy

Ho

Er

Tm

Yb

Lu

South America – rural and volcanic sediment, <5 μm

4

Bahia San Sebastian, Southern Patagonia

5.89

14.2

1.64

6.38

1.35

0.307

1.28

0.191

1.07

0.220

0.646

0.0890

0.585

0.0900

32

Rio Santa Cruz, El Calafate, Southern Patagonia

32.4

100

9.91

41.3

9.42

2.16

9.53

1.45

7.96

1.57

4.72

0.636

4.26

0.609

42

Punta Arenas, Southern Patagonia

6.14

12.7

1.45

5.22

1.13

0.309

1.06

0.187

1.17

0.264

0.838

0.133

0.948

0.153

CH

Chaiten Volcano, Southern Volcanic Zone

24.6

48.4

5.25

17.5

2.96

0.529

2.44

0.377

2.09

0.428

1.38

0.210

1.48

0.230

PU2

Puyehue Volcano, Southern Volcanic Zone

29.7

71.6

8.94

36.9

8.39

1.58

8.74

1.44

8.66

1.85

5.89

0.880

6.16

0.924

Reference Material

USGS G-2

This study (n=12)

86.7

158

15.9

52.4

7.19

1.34

4.00

0.459

2.16

0.353

0.853

0.113

0.696

0.0908

RSD (%)

0.7

0.6

1.5

1.1

1.2

1.8

2.1

2.0

2.7

2.5

1.9

2.8

12.0

2.2

USGS G-2

Reference values

87

158

16.3

51.5

6.8

1.41

4.1

0.49

2.08

0.35

0.88

0.117

0.72

0.12

RSD (%)

2.8

1.6

3.0

2.2

2.1

5.0

4.0

8.6

25

3.8

5.1

4.4

5.8

13

Table S3. (continued.)

Sample ID

Sample Location

Cu

Pb

Cd

Zn

Cr

Ni

Th

Co

Y

V

Sc

South America

Rural – Topsoil, Bed sediment (bulk)

4

Bahia San Sebastian, Southern Patagonia

10.8

4.25

0.137

46.8

13.0

6.4

2.31

4.67

7.44

38.7

4.93

5

Bahia San Sebastian, Southern Patagonia

7.00

11.4

0.0541

69.3

42.0

14.0

7.20

8.55

19.2

100

12.7

8

Bahia San Sebastian, Southern Patagonia

7.44

13.0

0.0472

83.9

51.5

18.9

8.41

10.5

21.5

122

15.3

9

Bahia San Sebastian, Southern Patagonia

9.74

14.7

0.0630

76.0

43.8

16.8

7.49

10.9

21.2

115

14.1

10

Bahia San Sebastian, Southern Patagonia

9.85

14.2

0.0677

84.4

49.6

18.0

7.88

10.9

20.2

130

14.9

11

Bahia San Sebastian, Southern Patagonia

10.1

13.9

0.0527

83.2

46.7

17.4

7.74

11.0

20.3

116

14.4

12

Bahia San Sebastian, Southern Patagonia

6.15

10.8

0.0413

68.1

44.4

15.3

7.55

8.29

21.1

106

13.9

19

Rio Gallegos, Southern Patagonia

22.7

16.7

0.0655

71.9

39.4

9.3

7.28

8.13

9.18

84.0

13.9

21

Rio Gallegos, Southern Patagonia

12.6

8.12

0.0799

69.2

42.5

13.5

4.56

12.2

16.3

114

16.5

35

Rio Santa Cruz, Southern Patagonia

14.9

10.9

0.0935

72.6

27.1

18.3

5.89

13.3

21.1

109

14.6

40

Punta Arenas, Southern Patagonia

22.3

9.86

<0.0015

55.4

30.5

22.0

3.90

18.8

7.72

105

12.2

42

Punta Arenas, Southern Patagonia

19.4

13.5

0.0823

65.3

29.7

10.1

4.35

7.04

8.24

106

11.3

1

Rio Grande, Southern Patagonia

9.79

10.6

0.0861

67.0

38.7

12.4

6.76

7.73

19.9

94.8

12.3

2

Rio Grande, Southern Patagonia

9.78

11.2

0.0870

69.7

41.6

14.1

7.65

8.56

20.8

105

13.0

13

Rio Grande, Southern Patagonia

11.8

12.5

0.0607

68.9

45.0

12.8

7.64

5.32

21.8

104

13.4

15

Rio Grande, Southern Patagonia

8.11

9.49

0.0399

56.8

39.6

13.2

6.14

8.35

20.4

89.0

12.6

17

Rio Grande, Southern Patagonia

7.92

7.00

0.0364

48.2

34.0

13.3

4.92

8.28

20.7

88.2

12.4

24

Rio Grande, Southern Patagonia

6.76

8.45

0.0444

49.6

32.4

11.9

5.05

8.00

17.1

80.7

10.6

27

Bahia Grande, Southern Patagonia

3.71

6.27

0.0337

39.0

66.9

10.5

4.83

7.43

14.5

66.7

10.1

Table S3. (continued.)

Sample ID

Sample Location

Cu

Pb

Cd

Zn

Cr

Ni

Th

Co

Y

V

Sc

Rural – Topsoil, Bed sediment (bulk)

28

Bahia Grande, Southern Patagonia

16.7

10.5

0.0784

64.9

54.0

19.9

5.95

11.0

17.1

102

13.8

30

Rio Santa Cruz, El Calafate, Southern Patagonia

10.5

12.9

0.0467

56.8

38.4

10.8

8.24

8.83

22.6

76.4

12.5

32

Rio Santa Cruz, El Calafate, Southern Patagonia

8.12

11.8

0.0474

55.3

28.5

11.2

6.90

7.39

21.9

76.8

11.5

33

Rio Santa Cruz, El Calafate, Southern Patagonia

10.3

10.5

0.0821

56.2

13.7

11.7

5.92

8.39

18.4

78.5

10.7

38

Argentino Lake, El Calafate, Southern Patagonia

18.1

9.87

0.0989

65.1

47.1

18.4

7.11

11.9

17.9

99.1

12.8

Volcanic – Volcanic clasts and tephra (bulk)

CH

Chaiten Volcano, Southern Volcanic Zone

2.81

19.2

0.0612

33.7

0.974

0.343

12.9

1.19

12.0

3.30

2.31

PU1

Puyehue Volcano, Southern Volcanic Zone

17.8

16.5

0.192

83.8

0.606

0.409

0.482

3.66

48.0

15.3

18.3

PU2

Puyehue Volcano, Southern Volcanic Zone

15.6

17.4

0.194

82.7

1.45

0.477

0.473

3.78

47.1

17.7

18.2

PU3

Puyehue Volcano, lakeside near La Angostura

13.6

18.8

0.140

80.8

0.329

0.268

0.346

2.25

41.8

6.36

15.2

CO

Cotopaxi Volcano, Northern Volcanic Zone

21.4

7.12

0.108

89.3

41.3

25.4

0.185

27.0

13.8

216

25.4

Urban – Road dusts (50-100μm)

3C

Urban Area, Buenos Aires

234

244

0.999

519

66.2

23.3

8.52

7.71

17.9

52.8

6.70

9C

Urban Area, Buenos Aires

231

482

0.796

643

113

32.7

12.6

8.86

21.2

72.8

7.94

110C

Urban Area, Buenos Aires

794

489

1.73

1000

117

58.6

10.5

9.42

19.3

63.3

7.26

112C

Urban Area, Buenos Aires

944

569

1.79

1306

144

174

17.9

18.2

17.7

55.1

6.50

3D

Urban Area, Buenos Aires

298

269

0.819

422

79.0

19.2

12.6

7.25

16.3

46.3

5.60

9D

Urban Area, Buenos Aires

142

426

0.624

535

81.2

21.7

14.5

7.32

15.6

43.9

5.90

110D

Urban Area, Buenos Aires

1623

547

1.25

1199

116

46.0

12.7

9.35

15.0

52.4

5.44

Table S3. (continued.)

Sample ID

Sample Location

Cu

Pb

Cd

Zn

Cr

Ni

Th

Co

Y

V

Sc

Urban – Aerosols (<10μm)

112D

Urban Area, Buenos Aires

627

407

1.75

993

96.5

44.3

11.2

8.70

17.4

58.7

6.87

648

Urban Area, São Paulo

93.7

97.1

4.50

584

146

25.2

0.619

2.08

40.4

40.4

0.437

649

Urban Area, São Paulo

42.2

133

5.54

990

n.d.

17.0

2.02

6.90

14.6

650

Urban Area, São Paulo

220

270

13.1

1357

278

53.2

0.716

9.48

34.5

34.5

0.705

Southern Africa

Rural – Lichen

PILA

Rural Area, Johannesburg

11.7

6.07

0.0613

30.3

202

12.7

0.876

1.96

1.88

7.17

0.885

Urban – Lichen

RIV

Urban Area, Johannesburg

23.5

68.7

0.295

84.5

147

8.99

1.07

1.59

2.48

11.1

1.37

DEL

Urban Area, Johannesburg

33.0

108

0.212

80.6

196

14.4

1.64

2.56

3.81

17.2

1.99

CMG

Urban Area, Johannesburg

20.6

71.0

0.322

121

91.8

10.9

1.21

2.34

2.81

11.6

1.54

EMER

Urban Area, Johannesburg

44.1

93.7

0.292

80.5

119

12.3

1.41

2.67

3.09

13.6

1.71

HUDD

Urban Area, Johannesburg

20.1

46.9

0.149

94.3

116

10.4

1.33

1.69

2.76

11.0

1.46

BOT2

Urban Area, Johannesburg

18.5

52.5

0.158

72.8

156

10.8

1.15

1.75

2.22

11.2

1.27

Mine – Tree bark

DRD-TB

Mine Dump Site, Johannesburg

6.92

9.53

0.121

31.6

26.4

7.14

0.373

5.72

1.11

3.36

0.459

Table S3. (continued.)

Sample ID

Sample Location

Cu

Pb

Cd

Zn

Cr

Ni

Th

Co

Y

V

Sc

South America – rural and volcanic sediment, <5 μm

4

Bahia San Sebastian, Southern Patagonia

10.9

4.71

0.146

68.0

9.76

6.04

5.59

36.4

4.09

5.85

1.68

32

Rio Santa Cruz, El Calafate, Southern Patagonia

19.5

24.1

0.098

130

45.0

30.4

14.7

147

22.0

43.6

10.6

42

Punta Arenas, Southern Patagonia

28.8

18.8

0.082

96.7

45.4

13.0

9.09

159

12.6

6.60

5.85

CH

Chaiten Volcano, Southern Volcanic Zone

3.83

20.5

0.069

47.1

3.63

1.44

1.72

9.00

2.95

13.3

13.0

PU2

Puyehue Volcano, Southern Volcanic Zone

13.2

24.9

0.190

83.8

0.521

0.404

3.05

8.40

11.5

52.8

8.88

Reference Material

USGS G-2

This study (n=12)

9.12

31.6

0.0242

86.1

7.63

2.15

23.8

4.48

9.10

35.1

4.69

RSD (%)

6.0

1.6

22.8

4.3

7.6

9.4

1.2

1.8

1.6

2.3

4.8

USGS G-2

Reference values

8.50

29

0.016

85

8.7

2

23.5

4.5

9.4

38

3.8

RSD (%)

6.6

5.4

6.3

3.1

25

5.2

3.6

4.4

3.5

3.4

4.7

The reference values for the USGS G-2 Granite reference material are from Gladney et al. (1992) for Cd and Cr, from Dulski (2001) for the REE, Y and Th, and from Pretorius et al. (2006) for all other elements. The precision of our G-2 data is 1x relative standard deviation (RSD) calculated from the results of multiple individual analyses (n = 12).

n.d. = not determined.

Table S4. Lead and Nd isotope compositions and εNd values for samples from South America and Southern Africa

Sample ID

Sample Location

206Pb

207Pb

±2SE

208Pb

207Pb

±2SE

206Pb

204Pb

±2SE

207Pb

204Pb

±2SE

208Pb

204Pb

±2SE

144Nd

143Nd

±2SE

εNd

South America

Rural – Topsoil, Bed sediment (bulk)

4

Bahia San Sebastian, Southern Patagonia

1.1967

0.0001

2.4681

0.0001

18.696

0.001

15.623

0.002

38.560

0.005

0.512669

0.000029

0.6

5

Bahia San Sebastian, Southern Patagonia

1.2004

0.0002

2.4744

0.0004

18.781

0.007

15.645

0.009

38.713

0.028

0.512477

0.000014

-3.1

8

Bahia San Sebastian, Southern Patagonia

1.1902

0.0002

2.4641

0.0004

18.614

0.007

15.639

0.009

38.536

0.029

0.512463

0.000018

-3.4

9

Bahia San Sebastian, Southern Patagonia

1.1936

0.0003

2.4671

0.0005

18.668

0.008

15.640

0.010

38.586

0.033

0.512486

0.000018

-3.0

10

Bahia San Sebastian, Southern Patagonia

1.1988

0.0003

2.4726

0.0006

18.755

0.009

15.640

0.012

38.684

0.038

0.512505

0.000012

-2.6

11

Bahia San Sebastian, Southern Patagonia

1.1998

0.0001

2.4731

0.0001

18.771

0.002

15.645

0.003

38.691

0.007

0.512488

0.000011

-2.9

12

Bahia San Sebastian, Southern Patagonia

1.2000

0.0001

2.4740

0.0001

18.776

0.001

15.647

0.001

38.711

0.001

0.512477

0.000010

-3.1

19

Rio Gallegos, Southern Patagonia

1.1983

0.0002

2.4714

0.0004

18.725

0.004

15.626

0.006

38.620

0.021

0.512599

0.000017

-0.1

21

Rio Gallegos, Southern Patagonia

1.1978

0.0001

2.4717

0.0003

18.722

0.001

15.631

0.003

38.639

0.008

0.512623

0.000015

-0.3

35

Rio Santa Cruz, Southern Patagonia

1.1995

0.0001

2.4723

0.0001

18.757

0.003

15.637

0.003

38.663

0.009

0.512598

0.000014

-0.8

40

Punta Arenas, Southern Patagonia

1.1870

0.0001

2.4590

0.0003

18.534

0.001

15.615

0.003

38.397

0.008

0.512814

0.000026

3.4

42

Punta Arenas, Southern Patagonia

1.1960

0.0001

2.4695

0.0001

18.697

0.002

15.632

0.003

38.605

0.009

0.512561

0.000022

-1.5

1

Rio Grande, Southern Patagonia

1.1962

0.0003

2.4696

0.0006

18.707

0.010

15.639

0.012

38.622

0.038

0.512461

0.000035

-3.5

2

Rio Grande, Southern Patagonia

1.1978

0.0002

2.4713

0.0004

18.737

0.006

15.644

0.008

38.660

0.025

0.512448

0.000025

-3.7

13

Rio Grande, Southern Patagonia

1.2006

0.0001

2.4741

0.0002

18.772

0.002

15.636

0.003

38.686

0.005

0.512463

0.000010

-3.4

15

Rio Grande, Southern Patagonia

1.1968

0.0001

2.4695

0.0003

18.707

0.003

15.630

0.004

38.601

0.014

0.512540

0.000013

-1.9

17

Rio Grande, Southern Patagonia

1.1734

0.0001

2.4465

0.0001

18.327

0.002

15.618

0.002

38.212

0.008

0.512582

0.000020

-1.1

24

Rio Grande, Southern Patagonia

1.1967

0.0003

2.4707

0.0004

18.719

0.005

15.642

0.008

38.647

0.023

0.512559

0.000018

-1.5

Table S4. (continued.)

Sample ID

Sample Location

206Pb

207Pb

±2SE

208Pb

207Pb

±2SE

206Pb

204Pb

±2SE

207Pb

204Pb

±2SE

208Pb

204Pb

±2SE

144Nd

143Nd

±2SE

εNd

27

Bahia Grande, Southern Patagonia

1.1963

0.0001

2.4716

0.0003

18.701

0.001

15.632

0.008

38.636

0.008

0.512575

0.000021

-1.2

28

Bahia Grande, Southern Patagonia

1.1987

0.0001

2.4742

0.0003

18.748

0.005

15.640

0.005

38.698

0.018

0.512511

0.000021

-2.5

30

Rio Santa Cruz, El Calafate, Southern Patagonia

1.1967

0.0001

2.4739

0.0003

18.711

0.005

15.635

0.005

38.681

0.020

0.512576

0.000014

-1.2

32

Rio Santa Cruz, El Calafate, Southern Patagonia

1.1814

0.0001

2.4579

0.0002

18.461

0.002

15.627

0.002

38.410

0.008

0.512573

0.000017

-1.3

33

Rio Santa Cruz, El Calafate, Southern Patagonia

1.1969

0.0001

2.4746

0.0001

18.715

0.002

15.636

0.002

38.694

0.005

0.512570

0.000017

-1.3

38

Argentino Lake, El Calafate, Southern Patagonia

1.1967

0.0001

2.4745

0.0001

18.714

0.003

15.638

0.003

38.698

0.010

0.512544

0.000023

-1.8

Volcanic – Volcanic clasts and tephra (bulk)

CH

Chaiten Volcano, Southern Volcanic Zone

1.2026

0.0001

2.4780

0.0003

18.812

0.006

15.643

0.006

38.763

0.020

0.512586

0.000008

-1.0

PU1

Puyehue Volcano, Southern Volcanic Zone

1.1908

0.0001

2.4670

0.0002

18.601

0.003

15.621

0.004

38.538

0.013

0.512829

0.000009

3.7

PU2

Puyehue Volcano, Southern Volcanic Zone

1.1907

0.0001

2.4664

0.0003

18.590

0.008

15.612

0.008

38.505

0.027

0.512841

0.000010

4.0

PU3

Puyehue Volcano, lakeside near La Angostura

1.1891

0.0001

2.4656

0.0001

18.570

0.002

15.617

0.002

38.506

0.004

0.512831

0.000009

3.8

CO

Cotopaxi Volcano, Northern Volcanic Zone

1.2002

0.0001

2.4703

0.0003

18.765

0.002

15.635

0.003

38.623

0.011

0.512816

0.000010

3.5

Urban – Road dusts (50-100μm)

3C

Urban Area, Buenos Aires

1.1626

0.0001

2.4391

0.0001

18.158

0.001

15.619

0.001

38.094

0.003

0.511957

0.000010

-13.3

9C

Urban Area, Buenos Aires

1.1605

0.0001

2.4378

0.0001

18.141

0.002

15.631

0.003

38.104

0.007

0.511840

0.000009

-15.6

110C

Urban Area, Buenos Aires

1.1615

0.0001

2.4394

0.0001

18.154

0.001

15.629

0.001

38.126

0.003

0.511946

0.000009

-13.5

112C

Urban Area, Buenos Aires

1.1629

0.0001

2.4448

0.0001

18.187

0.002

15.639

0.002

38.233

0.007

0.511633

0.000009

-19.6

3D

Urban Area, Buenos Aires

1.1630

0.0001

2.4420

0.0001

18.165

0.003

15.618

0.003

38.128

0.046

0.511704

0.000010

-18.2

9D

Urban Area, Buenos Aires

1.1567

0.0001

2.4373

0.0001

18.084

0.001

15.633

0.001

38.100

0.005

0.511660

0.000009

-19.1

Table S4. (continued.)

Sample ID

Sample Location

206Pb

207Pb

±2SE

208Pb

207Pb

±2SE

206Pb

204Pb

±2SE

207Pb

204Pb

±2SE

208Pb

204Pb

±2SE

144Nd

143Nd

±2SE

εNd

Urban – Aerosols (<10μm)

110D

Urban Area, Buenos Aires

1.1630

0.0001

2.4425

0.0001

18.190

0.002

15.640

0.002

38.200

0.007

0.511785

0.000017

-16.6

112D

Urban Area, Buenos Aires

1.1636

0.0001

2.4430

0.0001

18.186

0.001

15.629

0.002

38.182

0.005

0.511940

0.000015

-13.6

624

Urban Area, São Paulo

1.1887

0.0001

2.4472

0.0002

18.634

0.003

15.676

0.002

38.364

0.008

0.511852

0.000017

-15.3

648

Urban Area, São Paulo

1.1645

0.0002

2.4299

0.0003

18.192

0.012

15.621

0.012

37.959

0.032

n.d.

n.d.

n.d.

649

Urban Area, São Paulo

1.1592

0.0002

2.4265

0.0004

18.096

0.004

15.615

0.014

37.879

0.008

n.d.

n.d.

n.d.

650

Urban Area, São Paulo

1.1646

0.0001

2.4354

0.0002

18.189

0.006

15.618

0.003

38.036

0.009

n.d.

n.d.

n.d.

681

Urban Area, São Paulo

1.1829

0.0002

2.4333

0.0003

18.518

0.012

15.655

0.012

38.092

0.032

0.511915

0.000019

-14.1

Southern Africa

Rural – Lichen

PILA

Rural Area, Johannesburg

1.1380

0.0001

2.4043

0.0002

17.773

0.002

15.617

0.003

37.547

0.007

0.511610

0.000015

-20.1

Urban – Lichen

RIV

Urban Area, Johannesburg

1.0936

0.0001

2.3573

0.0001

17.002

0.003

15.547

0.003

36.650

0.009

0.511527

0.000014

-21.7

DEL

Urban Area, Johannesburg

1.0926

0.0001

2.3574

0.0001

16.968

0.002

15.531

0.002

36.613

0.007

0.511596

0.000012

-20.3

CMG

Urban Area, Johannesburg

1.1162

0.0001

2.3568

0.0004

17.394

0.005

15.583

0.007

36.727

0.021

0.511585

0.000017

-20.5

EMER

Urban Area, Johannesburg

1.0956

0.0001

2.3596

0.0002

17.019

0.002

15.534

0.003

36.653

0.009

0.511564

0.000013

-21.0

HUDD

Urban Area, Johannesburg

1.1058

0.0001

2.3692

0.0003

17.191

0.004

15.546

0.005

36.833

0.015

0.511646

0.000017

-19.4

BOT2

Urban Area, Johannesburg

1.0939

0.0017

2.3590

0.0004

16.984

0.066

15.526

0.037

36.679

0.107

0.511565

0.000015

-20.9

Mine – Tree bark

DRD-TB

Mine Dump Site, Johannesburg

1.3133

0.0002

2.2866

0.0003

21.186

0.007

16.132

0.007

36.886

0.022

0.511306

0.000018

-26.0

Table S4. (continued)

Sample ID

Sample Location

206Pb

207Pb

±2SE

208Pb

207Pb

±2SE

206Pb

204Pb

±2SE

207Pb

204Pb

±2SE

208Pb

204Pb

±2SE

144Nd

143Nd

±2SE

εNd

South America – rural and volcanic sediment, <5 μm

4

1.1946

0.0001

2.4695

0.0001

18.683

0.001

15.639

0.001

38.619

0.003

0.512672

0.000018

0.7

32

1.1942

0.0001

2.4739

0.0001

18.699

0.001

15.658

0.001

38.736

0.003

0.512616

0.000015

-0.4

42

1.1965

0.0001

2.4702

0.0001

18.709

0.001

15.637

0.001

38.627

0.003

0.512548

0.000023

-1.8

CH

1.2031

0.0001

2.4781

0.0002

18.816

0.003

15.640

0.003

38.758

0.011

0.512618

0.000013

-0.4

PU2

1.1892

0.0001

2.4653

0.0001

18.577

0.001

15.621

0.001

38.510

0.003

0.512868

0.000014

4.5

Reference Material

±2SD

±2SD

±2SD

±2SD

±2SD

±2SD

USGS G-2

This study (n=22)

1.1764

0.0010

2.4873

0.0007

18.399

0.016

15.640

0.014

38.902

0.044

0.512230

0.000025

-8.0

USGS G-2

Weis et al. (2006)

1.1765

0.0002

2.4878

0.0002

18.396

0.023

15.636

0.005

38.900

0.019

0.512235

0.000015

-8.0

The quoted 2SE ‘within-run’ precision quoted for samples is 2x standard error of the mean calculated from the individual cycles of each run.

The quoted precision for the USGS G-2 Granite reference material is the 2SD ‘external’ precision calculated from the results of multiple sample runs, for both the data of this study and the literature values of Weis et al. (2006).

n.d. = not determined. εNd values are reported relative to a CHUR value of 0.512638.