Supplementary material
Table S1. Description of Chemical Transport Models (CTM) used as data source
Data source
Description
EMEP MSCE-HM model
Regional heavy metal transport model (MSCE-HM)
Developer: Meteorological Synthesizing Centre - East (MSC-E)
Model type: Eulerian 3D grid model
Input:
Atmospheric emissions, meteorological information, geophysical
data (land cover data, leaf area index, oceanological input data)
Output:
Heavy metals (Cd, Pb, Hg)
Domain:
35° West to 60° East and from the North Pole to about 20° North
Spatial resolution: 50 x 50 km (Europe)
References: Travnikov O., Ilyin I. (2005) Regional Model MSCE-HM of Heavy
Metal Transboundary Air Pollution in Europe. EMEP/MSC-E
Technical Report 6/2005, p.59.
Tørseth K, Aas W, Breivik K, Fjæraa M, Fiebig M, Hjellbrekke, AG,
Lund Myhre C, Solberg S, Yttri KE (2012) Introduction to the
European Monitoring and Evaluation Programme (EMEP) and
observed atmospheric composition change during 1972-2009.
Atmos Chem Phys 12:5447-5481
LOTOS-EUROS (LE)
LOng Term Ozone Simulation - EURopean Operational Smog model
Developer: TNO Institute of Environmental Sciences, Utrecht, Netherlands
Model type: Eulerian 3D grid model
Input:
Anthropogenic emissions, 3-hourly meteorological data,
topography (tree species coverage, land cover data)
Output:
Oxidants (O3, VOCs, NOx, HNO3 etc.); Secondary Inorganic
Aerosol (SO4, NO3, NH4); Secondary Organic Aerosols (SOA) from
terpenes; Primary aerosol (PM2.5; PM10, Black Carbon, sea salt);
Heavy metals (Cd, Pb and other non-volatiles metals); Persistant
Organic Pollutants (POPs)
Domain:
35° and 70° North and 10° West and 60° East
Spatial resolution: 25 x 25 km (Europe); 7 x 7 km (national level)
References: Schaap, M., Roemer, M., Sauter, F., Boersen, G., Timmermans,
R., Builjes, P.J.H., Vermeulen, A.T. (2005) LOTOS-EUROS:
Documentation, TNO report B&O-A R 2005/297.
Schaap, M., Timmermans, R., Roemer, M., Boersen, G., Builjes,
P.J.H. (2008) The LOTOS–EUROS model: description, validation
and latest developments. Int. J. Environment and Pollution, Vol.
32, No. 2:270-290.
European Topic Centre on Air and Climate Change (ETC/AAC)
(2010) Long description of model 'LOTOS-EUROS. http://pandora.
meng.auth.gr/mds/showlong.php?id=57 (23.11.2015).
Table S2. Description of Biomonitoring programmes used as data source
Data source
Description
European Moss Survey (EMS)
International Cooperative Programme on the effects of air
pollution on natural vegetation and crops (ICP Vegetation) - Monitoring of
atmospheric deposition of heqavy metals, nitrogen and POPs in Europe using
bryophytes
Time period: 1990 – now
Indicators (used): HM concentration in moss
Ecosystem types: terrestrial ecosystems (preferably open landscape)
Analytes (HM): As, Cd, Co, Cr, Cu, Hg, Mn, Mo, Ni, Pb, Sb, Ti, V, and Zn
No. of plots: up to 7300 (Europe), 700-1000 (Germany)
Frequency: every 5 years (participating European countries)
References: ICP Vegetation (2014) Monitoring of atmospheric deposition of
heavy metals, nitrogen and POPs in Europe using bryophytes.
Monitoring manual 2015 survey. United Nations Economic
Commission for Europe Convention on Long-Range
Transboundary Air Pollution. ICP Vegetation Moss Survey
Coordination Centre, Dubna, Russian Federation, and Programme
Coordination Centre. Bangor, Wales, UK:1-26
iCP Forests Level II
International Co-operative Programme on Assessment and Monitoring of Air
Pollution Effects on Forests (iCP Forests) - Intensive monitoring
Time period: 1985 – now
Indicators (used): HM concentrations in tree foliage (leaves from beech (Fagus
sylvatica) and needles from spruce (Picea abies) and pine (Pinus
sylvestris)) and surface layers, respectively.
Ecosystem types: Major forest types of Europe
Analytes (HM): Cd, Cu, Mn, Pb, and Zn
No. of plots (foliar chemistry): 767 (Europe), up to 103 (Germany)
Frequency (foliar chemistry): every 2 years
References: Ferretti and Fischer (2013) Methods for terrestrial investigations in
Europe with an overview of North America and Asia.
Developments in environmental science 12. Elsevier,
Amsterdam:1-507
German Environmental Specimen
Bank (ESB)
Umweltprobenbank des Bundes (UPB)
Time period: 1987 – now
Indicators (used): Element concentrations in tree foliage (leaves from beech
(Fagus sylvatica) and poplar (Populus nigra 'Italica') and 1-year old
shoots from spruce (Picea abies) and pine (Pinus sylvestris)
Ecosystem types: terrestrial ecosystems (agrarian, urban-industrial, forestry and
nearly natural)
Analytes (HM): As, Cd, Co, Cr, Cu, Hg, Mo, Ni, Pb, Ti, and Zn
No. of plots (tree foliage): 10 (deciduous trees), 10 (conifers)
Frequency: annually
References: UBA (2008) Umweltprobenbank des Bundes – Konzeption (Stand:
Oktober 2008). Available at: http://www.umweltprobenbank.de/
upb_static/fck/download/Konzeption_Okt_2008_de.pdf
Table S3. Basic descriptive statistics of modelled total atmospheric deposition of Cd and Pb for 2005
and 2007-2011 referred to the 50 km by 50 km EMEP grids (N = 204) covering Germany
Variable
Cd deposition 2007, averaged over the land-use
classes (LOTOS-EUROS)
Cd deposition 2008, averaged over the land-use
classes (LOTOS-EUROS)
Cd deposition 2009, averaged over the land-use
classes (LOTOS-EUROS)
Cd deposition 2010, averaged over the land-use
classes (LOTOS-EUROS)
Cd deposition 2011, averaged over the land-use
classes (LOTOS-EUROS)
Pb deposition 2007, averaged over the land-use
classes (LOTOS-EUROS)
Pb deposition 2008, averaged over the land-use
classes (LOTOS-EUROS)
Pb deposition 2009, averaged over the land-use
classes (LOTOS-EUROS)
Pb deposition 2010, averaged over the land-use
classes (LOTOS-EUROS)
Pb deposition 2011, averaged over the land-use
classes (LOTOS-EUROS)
Cd deposition 2007, (EMEP)
Cd deposition 2008, (EMEP)
Cd deposition 2009, (EMEP)
Cd deposition 2010, (EMEP)
Cd deposition 2011, (EMEP)
Pb deposition 2007, (EMEP)
Pb deposition 2008, (EMEP)
Pb deposition 2009, (EMEP)
Pb deposition 2010, (EMEP)
Pb deposition 2011, (EMEP)
Mean = Arithmetic mean; SD= Standard deviation
Unit
Min
Max
Mean
Median
SD
µg/m² a
13.63
51.97
27.76
27.72
5.84
µg/m² a
13.39
50.13
25.28
24.63
5.32
µg/m² a
13.59
55.35
26.67
26.20
5.71
µg/m² a
15.50
57.15
29.11
28.21
6.54
µg/m² a
13.77
46.60
22.87
22.05
4.47
µg/m² a
322.17
1558.50
664.44
649.54
173.51
µg/m² a
316.90
1556.12
614.41
588.08
166.82
µg/m² a
322.64
1611.63
634.50
612.25
169.79
µg/m² a
379.52
1744.15
679.83
655.61
176.65
µg/m² a
332.01
1367.75
556.31
523.57
140.87
µg/m² a
µg/m² a
µg/m² a
µg/m² a
µg/m² a
µg/m² a
µg/m² a
µg/m² a
µg/m² a
µg/m² a
16.52
15.15
16.73
13.44
15.39
690.24
547.59
569.53
461.85
570.35
217.85
172.40
143.69
143.96
227.74
5154.91
3955.38
3285.66
3099.06
4941.32
50.95
39.42
37.10
35.71
43.41
1763.36
1225.53
1152.65
1076.22
1450.07
45.35
34.29
31.31
31.14
36.40
1649.47
1138.57
1045.74
1014.36
1336.82
24.49
19.46
17.85
18.24
25.82
656.05
445.10
424.74
401.12
581.23
Table S4. Basic descriptive statistics of measured concentrations of Cd and Pb in moss and in
respective total deposition modelled by use of EMEP and LE
Variable
Unit
Min
Max
Mean
Median
Cd conc. in moss 2005
(Germany)
Cd deposition 2005 (Germany),
averaged over land-use classes
(LOTOS-EUROS)
Cd deposition 2005 (Germany),
coniferous forest (LOTOS-EUROS)
Cd deposition 2005 (Germany),
deciduous forest (LOTOS-EUROS)
Cd deposition 2005 (Germany),
grassland (LOTOS-EUROS)
Cd deposition 2005 (Germany) (EMEP)
Cd deposition 2005 (Germany),
coniferous forest (EMEP)
Cd deposition 2005 (Germany),
deciduous forest (EMEP)
Cd deposition 2005 (Germany),
grassland (EMEP)
Cd conc. in moss 2005 (Europe)
Cd deposition 2005 (Europe),
averaged over land-use classes
(LOTOS-EUROS)
Cd deposition 2005 (Europe) (EMEP)
Pb conc. in moss 2005 (Germany)
Pb deposition 2005 (Germany),
averaged over land-use classes
(LOTOS-EUROS)
Pb deposition 2005 (Germany),
coniferous forest (LOTOS-EUROS)
Pb deposition 2005 (Germany),
deciduous forest (LOTOS-EUROS)
Pb deposition 2005 (Germany),
grassland (LOTOS-EUROS)
Pb deposition 2005 (Germany) (EMEP)
Pb deposition 2005 (Germany),
coniferous forest (EMEP)
Pb deposition 2005 (Germany),
deciduous forest (EMEP)
Pb deposition 2005 (Germany),
grassland (EMEP)
Pb conc. in moss 2005 (Europe)
Pb deposition 2005 (Europe),
averaged over land-use classes
(LOTOS-EUROS)
Pb deposition 2005 (Europe) (EMEP)
µg/g
0.06
1.71
0.24
0.20
0.14
µg/m² a
12.37
74.73
21.36
20.58
5.92
µg/m² a
11.13
101.64
25.83
24.51
7.11
µg/m² a
13.30
81.47
23.31
22.28
5.64
µg/m² a
9.52
56.52
17.66
16.92
4.14
µg/m² a
µg/m² a
21.66
26.61
98.13
1029.70
46.84
162.88
42.80
134.48
14.79
130.99
µg/m² a
23.92
759.91
119.25
98.02
95.46
µg/m² a
13.85
134.21
39.28
35.03
18.94
µg/g
µg/m² a
0.01
2.01
6.72
221.03
0.22
16.74
0.17
14.58
0.24
11.98
µg/m² a
µg/g
µg/m² a
3.45
1.19
310.81
701.88
40.41
2618.53
42.67
4.54
563.12
32.52
3.70
520.99
44.73
3.28
211.03
µg/m² a
304.00
3569.43
677.03
618.76
257.93
µg/m² a
329.94
2837.74
605.77
555.03
205.62
µg/m² a
262.60
1954.01
472.58
432.54
152.07
µg/m² a
µg/m² a
777.92
1039.4
3244.38
20691.0
1816.97
5214.85
1739.91
4616.10
535.79
2799.58
µg/m² a
907.22
15153.0
3792.73
3467.50
2040.68
µg/m² a
536.36
3651.60
1379.97
1258.50
495.15
µg/g
µg/m² a
0.10
49.79
248.64
2618.53
6.19
342.63
3.79
290.95
9.42
216.48
µg/m² a
115.44
5550.18
1233.65
1085.50
778.43
Mean = Arithmetic mean; SD= Standard deviation
SD
Table S5. Basic descriptive statistics of measured concentrations of As, Cr, Cu, Ni, V, and Zn in moss
and in respective total deposition modelled by use of LE
Variable
As conc. in moss 2005 (Germany)
As deposition 2009-2011 (Germany),
LOTOS-EUROS
Cr conc. in moss 2005 (Germany)
Cr deposition 2009-2011 (Germany),
LOTOS-EUROS
Cu conc. in moss 2005 (Germany)
Cu deposition 2009-2011 (Germany), LOTOSEUROS
Ni conc. in moss 2005 (Germany)
Ni deposition 2009-2011 (Germany),
LOTOS-EUROS
V conc. in moss 2005 (Germany)
V deposition 2009-2011 (Germany),
LOTOS-EUROS
Zn conc. in moss 2005 (Germany)
Zn deposition 2009-2011 (Germany),
LOTOS-EUROS
Unit
Min
Max
Mean
Median
SD
µg/g
µg/m² a
0.004
2.16
21.60
90.51
0.43
24.79
0.17
23.63
0.99
13.35
µg/g
µg/m² a
0.01
6.38
90.74
309.73
2.49
78.57
1.29
74.92
4.56
41.29
µg/g
µg/m² a
0.01
8.19
671.92
6939.07
6.92
273.49
5.34
188.83
14.14
247.91
µg/g
µg/m² a
0.03
14.69
1016.03
609.46
2.46
171.18
1.39
162.18
15.11
79.53
µg/g
µg/m² a
0.02
4.65
43.50
337.78
2.31
41.80
1.40
35.91
2.93
23.82
µg/g
µg/m² a
6.06
59.48
693.82
7054.55
36.94
1092.28
32.49
914.81
22.95
843.18
Mean = Arithmetic mean; SD= Standard deviation
Table S6. Basic statistical parameters for atmospheric Cd and Pb deposition modelled with EMEP and
LE for Europe and Germany and respective geostatistical surface estimations derived from EMS
Variable
Unit
Min
Max
Mean
Median
Cd conc. in moss 2005 (Germany),
geostatistically estimated
Cd deposition 2005 (Germany),
(LOTOS-EUROS)
Cd deposition 2005 (Germany),
(EMEP)
Pb conc. in moss 2005 (Germany),
geostatistically estimated
Pb deposition 2005 (Germany),
(LOTOS-EUROS)
Pb deposition 2005 (Germany),
(EMEP)
Cd conc. in moss 2005 (Europe)
geostatistically estimated
Cd deposition 2005 (Europe),
(LOTOS-EUROS)
Cd deposition 2005 (Europe),
(EMEP)
Pb conc. in moss 2005 (Europe)
geostatistically estimated
Pb deposition 2005 (Europe),
(LOTOS-EUROS)
Pb deposition 2005 (Europe),
(EMEP)
µg/g
0.06
0.60
0.23
0.21
0.06
µg/m² a
12.77
81.45
21.25
20.41
5.93
µg/m² a
22.82
98.13
45.69
42.38
13.82
µg/g
2.50
11.95
4.32
4.00
3.28
µg/m² a
330.32
2864.29
561.29
513.98
211.85
µg/m² a
820.73
3244.38
1779.87
1728.09
506.58
µg/g
0.01
1.85
0.20
0.16
0.15
µg/m² a
1.76
239.90
15.50
11.49
12.90
µg/m² a
3.48
722.69
38.78
30.76
37.33
µg/g
0.83
36.26
6.92
5.29
4.91
µg/m² a
42.53
2931.25
290.26
251.14
191.41
µg/m² a
114.21
5359.67
1074.24
949.05
647.76
Mean = Arithmetic mean; SD= Standard deviation
SD
Table S7. Basic statistical parameters for atmospheric As, Cr, Cu, Ni, V, and Zn deposition modelled
with LE for Germany and respective geostatistical surface estimations derived from EMS
Variable
Unit
Min
Max
Mean
Median
As conc. in moss 2005, (Germany),
geostatistically estimated
As deposition 2009-2011 (Germany),
LOTOS-EUROS
Cr conc. in moss 2005 (Germany),
geostatistically estimated
Cr deposition 2009-2011 (Germany),
LOTOS-EUROS
Cu conc. in moss 2005 (Germany),
geostatistically estimated
Cu deposition 2009-2011 (Germany),
LOTOS-EUROS
Ni conc. in moss 2005 Germany,
geostatistically estimated
Ni deposition 2009-2011 (Germany),
LOTOS-EUROS
V conc. in moss 2005 (Germany),
geostatistically estimated
V deposition 2009-2011 (Germany),
LOTOS-EUROS
Zn conc. in moss 2005 (Germany),
geostatistically estimated
Zn deposition 2009-2011 (Germany),
LOTOS-EUROS
µg/g
0.10
0.59
0.19
0.17
0.08
µg/m² a
21.43
84.81
34.74
32.88
8.69
µg/g
1.48
14.98
3.43
2.89
2.15
µg/m² a
64.68
309.73
121.82
111.47
39.38
µg/g
5.28
14.29
7.68
7.47
1.53
248.73
2165.10
577.24
537.79
61.87
0.73
2.32
1.32
1.27
0.32
143.20
609.46
246.31
233.30
61.87
µg/g
0.69
1.78
1.16
1.17
0.24
µg/m² a
25.96
172.27
41.28
36.61
16.64
µg/g
30.70
110.37
52.09
49.20
13.29
µg/m² a
925.51
6338.43
1844.08
1695.46
711.90
Mean = Arithmetic mean; SD= Standard deviation
µg/m² a
µg/g
µg/m² a
SD
Figure S1. Spatial patterns of ratios calculated from median values of atmospheric deposition of Cd and
Pb (2011) for grassland modelled by use of EMEP and LE
Figure S2. Spatial patterns of ratios calculated from median values of atmospheric deposition of Cd and
Pb (2011) for coniferous forests modelled by use of EMEP and LE
Figure S3. Spatial patterns of ratios calculated from median values of atmospheric deposition of Cd and
Pb (2011) for deciduous forests modelled by use of EMEP and LE
Figure S4. Spatial patterns of aggregated deviances of modelled deposition (LE, 2009-2011, left) and
concentrations in moss (2005, right) of As, Cd, Cr, Cu, Ni, Pb, V, and Zn from the respective Germanywide median
Figure S5. Deviations of LE modelled total As deposition (mean 2009-2011) (left) and As
concentrations in moss (2005) (right) from the respective Germany-wide median
Figure S6. Deviations of LE modelled total Cr deposition (mean 2009-2011) (left) and Cr concentrations
in moss (2005) (right) from the respective Germany-wide median
Figure S7. Deviations of LE modelled total Cu deposition (mean 2009-2011) (left) and Cu
concentrations in moss (2005) (right) from the respective Germany-wide median
Figure S8. Deviations of LE modelled total Ni deposition (mean 2009-2011) (left) and Ni concentrations
in moss (2005) (right) from the respective Germany-wide median
Figure S9. Deviations of LE modelled total V deposition (mean 2009-2011) (left) and V concentrations
in moss (2005) (right) from the respective Germany-wide median
Figure S10. Deviations of LE modelled total Zn deposition (mean 2009-2011) (left) and Zn
concentrations in moss (2005) (right) from the respective Germany-wide median