SUPPORTING INFORMATION Estimation of speciated and total mercury dry deposition at monitoring locations in eastern and central North America L. Zhang, P. Blanchard, D.A. Gay, E.M. Prestbo, M.R. Risch, D. Johnson, J. Narayan, R. Zsolway, T.M. Holsen, E.K. Miller, M.S. Castro, J.A. Graydon, V.L. St. Louis, J. Dalziel Contents Table S. Population density within the 5km radius circle surrounding each site and defined site categories. Also shown in the last column is the fraction of each land use category (LUC) within the km circle surrounding each site (number in brackets are LUC number defined in Zhang et al., (23). Table S2. Litterfall measurements collected at selected MDN sites. Table S3. Seasonal averages ±standard deviation of speciated Hg ambient concentrations (GEM in ng m -3 and GOM and PBM in pg m -3 ) from monitoring data collected during the years of 28 and 29. Spring: Mar., Apr. and May; Summer: Jun., Jul. and Aug.; Fall: Sep., Oct. and Nov.; Winter: Dec., Jan. and Feb. Figure S. Seasonal average concentrations for (a) GOM (pg m -3 ), (b) PBM (pg m -3 ) and (c) GEM (ng m -3 ). Figure S2. Average diurnal cycle and monthly V d (left columns) and normalized V d by their respective annual average V d (right columns) from 29 data at Kejimkujik forest site.
Table S. Population density within the 5km radius circle surrounding each site and defined site categories. Also shown in the last column is the fraction of each land use category (LUC) within the km circle surrounding each site (number in brackets are LUC number defined in Zhang et al., (23). AMNet Site Site Name Grid count Area (km²) Max / km² Mean / km² Std / km² Site category Fraction of each LUC with km circle. LUC number in ID bracket. MD8 Piney Reservoir 4 72 85 37 28 rural.(3),.25(7),.5(),.(2),.(3),.4(4) MD99 Beltsville 42 729 923 326 28 suburban.36(5),.89(7),.34(),.2(4),.344(2),.22(25) MS2 Grand Bay NERR 39 677 356 336 655 rural.2(),.37(5),.4(),.4(3),.423(2),.32(2) NH6 Thompson Farm 43 747 78 524 4 rural.5(),.5(3),.3(3),.25(5),.2(23),.77(25) NJ5 Brigantine 43 747 6243 649 233 subrural.239(3),.63(4),.34(7),.3(5),.28(2),.46,(23),.27(25) NJ3 New Brunswick 42 729 928 4 247 urban.82(3),.24(7),.249(5),.438(2),.8(23) NJ32 Chester 42 729 5784 5 927 suburban.23(7),.3 (),.47(5),.565(2),.5(23),. (24) NJ54 Elizabeth Lab 39 677 32464 274 7 urban.42 (3),.28(),.889(2),.4(23) NS Kejimkujik 42 729 2 7 3 rural.67(4),.33(25) National Park NY6 Bronx 42 729 83589 888 2433 urban.5(7).95(2) NY2 Huntington Wildlife 44 764 6 3 rural.4(3),.5(23),.45(25) NY43, NY95 Rochester 42 729 854 2859 2638 suburban.(2) OH2 Athens Super Site 42 729 298 238 454 rural.4(7),.(),.25(3),.25(25) OK99 Stilwell 42 729 44 63 67 rural.5(),.2(5),.28(7),.4(),.4(3),.67(4),.43(2),.2(24),.5(25) UT96 Antelope Island 44 764 485 8 448 suburban.3(),.627(4),.279(5),.72(2),.9(2) UT97 Salt Lake City 42 729 67 3827 3323 urban.4(),.4(),.(4),.(2),.972(2) VT99 Underhill 45 78 48 8 7 rural.5(),.5(4),.3(7),.(),.2(3),.2(4) WV99 Canaan Valley 4 72 3 6 3 rural.3 (),.97 (25) Institute Experimental Lakes Area 5 868 rural.25(4),.75(25) (i) The population estimates are from the 2 Gridded Population of the World - GPW v3 database prepared by the Center for International Earth Science Information Network (CIESIN), Columbia University; and Centro Internacional de Agricultura Tropical (CIAT), 25. http://sedac.ciesin.columbia.edu/gpw/ (ii) Grid and Area: number of population grid cells and their total area used for statistics calculation; the original grids are ~ 4.64 km x 4.64 km. (iii) Definition of LUC number:. water; 2. ice; 3. inland lake; 4. evergreen needleleaf trees; 5. evergreen broadleaf trees; 6. deciduous needleleaf trees; 7. deciduous broadleaf trees; 8. tropical broadleaf trees; 9. drought deciduous trees;. evergreen broadleaf shrubs;. deciduous shrubs; 2. thorn shrubs; 3. short grass and forbs; 4. long grass; 5. crops; 6. rice; 7. sugar; 8. maize; 9. cotton; 2. irrigated crops; 2. urban; 22. tundra; 23. swamp; 24. desert; 25. mixed wood forests; 26. transitional forest.
Table S2. Litterfall measurements collected at selected MDN sites following from Risch et al., 22a. MDN site number Site name Latitude Longitude Elevation (m) Co-located monitoring a at MDN site Prevalent tree species in study plot Forest cover class of study plot National Land Cover Database b class for study plot Annual litterfall deposition ( g/m 2 ) GA9 Okefenokee 3.74-82.3 47 NTN pine, oak mixed transitional 5.4 ±. IN2 Roush Lake 4.84-85.46 244 NTN maple, poplar, ash, cherry deciduous row crops 3.9 ± 5.2 IN2 Clifty Falls 38.76-85.42 256 none maple, poplar, ash deciduous forest and residential 6. ±.2 IN26 Fort Harrison 39.86-86.2 26 none oak, maple, poplar, cherry deciduous urban 7.4 ± 5.5 IN34 Indiana Dunes 4.63-87.9 28 NTN oak, maple, hickory deciduous pasture 8.7 ± 5.7 KY Mammoth Cave 37.3-86.5 236 NTN oak, maple, hickory, ash deciduous pasture 2.6 ±. MD8 Piney Reservoir 39.7-79. 769 NTN, AMNet oak, maple, cherry deciduous deciduous forest 5.3 ± 2. MD99 Beltsville 39.3-76.82 46 NTN, AMNet oak, maple, beech, sweetgum deciduous urban 5.5 ±. MI48 Seney 46.29-85.95 26 NTN red pine, jack pine, balsam fir, birch coniferous woody wetland 7.4 ±.4 MN6 Marcell 47.53-93.47 43 NTN aspen, maple deciduous deciduous forest 3.8 ±.4 MN98 Blaine 45.4-93.22 275 none aspen, maple deciduous not determined 7.8 ±.3 NY68 Biscuit Brook 4.99-74.5 634 NTN, CASTNET beech, maple deciduous deciduous forest 5.3 ±. OH2 Athens 39.3-82.2 275 AMNet oak, maple, hickory, cherry deciduous pasture 8.8 ± 2.8 PA3 Allegheny Portage 4.46-78.56 739 none oak, maple, beech, cherry deciduous commercial industrial 3.6 ± 4. SC5 Cape Romaine 32.94-79.66 3 NTN oak, hickory, sweetgum, pine mixed residential 9.3 ±.2 TN Smoky Mountains 35.66-83.59 64 NTN, CASTNET maple, poplar, birch, pine, hemlock deciduous mixed forest 4.9 ± 4.7 VA28 Shenandoah 38.52-78.44,74 NTN, CASTNET birch, locust, oak, pine mixed deciduous forest 7.8 ±.8 VT99 Underhill 44.53-72.87 399 NTN, AMNet, AirMon birch, maple, beech, hemlock, spruce mixed deciduous forest.3 ±.8 WI9 Popple River 45.8-88.4 42 NTN birch, maple, aspen, fir mixed herbaceous wetland. ±. WI3 Devil's Lake 43.44-89.68 389 none cottonwood, maple, oak, elm deciduous pasture 4.6 ±. WI36 Trout Lake 46.5-89.65 5 NTN pine, fir, spruce coniferous evergreen forest 7.6 ±.4 WI99 Lake Geneva 42.58-88.5 288 NTN oak, basswood, ash, elm deciduous deciduous forest 4.3 ±.3 WV99 Canaan Valley 39.6-79.42 988 AMNet birch, maple, beech, hemlock, spruce mixed pasture 9.9 ±.3 a MDN, Mercury Deposition Network; NTN, National Trends Network; AMNet, Atmospheric Mercury Network; CASTNET, Clean Air Status and Trends Network; AirMon, Atmospheric Integrated Research Monitoring Network. b Multi-Resolution Land Characteristics Consortium (2).
Table S3. Seasonal averages ±standard deviation of speciated Hg ambient concentrations (GEM in ng m -3 and GOM and PBM in pg m -3 ) from monitoring data collected during the years of 28 and 29. Spring: Mar., Apr. and May; Summer: Jun., Jul. and Aug.; Fall: Sep., Oct. and Nov.; Winter: Dec., Jan. and Feb. GEM GOM PBM Site Code Spring Summer fall winter Spring Summer fall winter Spring Summer fall winter MD8.54 ±.9.25 ±.26.2 ±.9.54 ±.2 35.88 ± 34.79 9.95 ±.88 9.2 ± 29 22.7 ± 3.9 8.9 ± 6.8 3.2 ± 2.3 4.2 ± 3.6.35 ± 9.29 MD99.5 ±.22.39 ±.24.98 ±.7.34 ±.7 5.4 ± 7.4 3.6 ± 8..46 ± 2.85 ± 4.55 7.54 ± 6.26 5.35 ± 3.88.65 ±.2 6.4 ± 8.75 MS2.45 ±.27.36 ±.7.29 ±.4.45 ±.33 8.9 ± 22.2 9.53 ± 6.54 6.46 ±.26 4.53 ±.26 3.24 ± 3.42 2.79 ± 5.85 5.4 ± 8.85 5.59 ± 6.27 NH6.5 ±.4.26 ±.2.5 ±.5.39 ±.8 5.5 ± 6.68.58 ± 2.68.49 ±.82 3.42 ± 3.54 4.24 ± 5.28 2.45 ±.74.85 ±.2 4.25 ± 4.56 NJ5.76 ±.59.35 ±.3.45 ±.8 22.7 ±.8.3 ±.65.4 ±.98 2 ± 2.57.98 ± 2.56 4.68 ± 4.5 NJ3 2.3 ±.35 2.25 ±.35.82 ±.23 3.5 ± 6.27.79 ± 2.65.59 ± 2.6.2 ± 8.8 3.66 ± 4.99 3.55 ± 6.93 NJ32.98 ±.77.97 ±.77.38 ±.25.22 ±.36 8.57 ± 9.92 2.76 ± 3.63 4.93 ± 9.8 9.29 ±.2 9.3 ± 2.3 5.2 ± 8.24.82 ± 4.7 4.29 ± 34.86 NJ54.78 ±.64.67 ±.48.6 ±.2.9 ±.63 8.7 ±.57 2.48 ±.59 5.68 ± 6.5 5.48 ± 5.83 6.57 ± 4.4 5.6 ± 4.3 7.65 ± 26.37 9.85 ± 4.24 NS.58 ±.35.27 ±.26.7 ±.22.45 ±.9 4.9 ± 6.22 2.86 ± 3.55.53 ±.58.49 ±.33 7.98 ± 8..76 ±.3.28 ±.2 5.8 ± 4.87 NY6.62 ±.29.58 ±.38.4 ±.34.43 ±.39.68 ± 5.87 7.62 ± 8.68 5.2 ± 5.97 3.69 ± 3.29 9.3 ± 7.4 4.97 ± 4.8 5.3 ± 5.4.93 ±.93 NY2.3 ±.35.25 ±.3.37 ± 3..6 ±.5.59 ± 3.33.7 ± 2.52.53 ±.6.42 ± 4.3 2.49 ± 3.6.65 ± 3.6.92 ± 2.5 7.6 ± 4.3 NY43.56 ±.65.52 ±.3.49 ±.35.72 ±.29 3.74 ± 9 3.8 ± 5.73 2.76 ± 5.23 3.92 ± 5.69.6 ± 8.34 5.59 ± 3.79 4.67 ± 5.47 6.5 ± 4.9 NY95.49 ±.7.38 ±.9.38 ±.6.47 ±.5.5 ± 5.39 5.4 ± 6.5 2.7 ±.59 6.88 ± 7.77.35 ± 6.99 6. ± 3.33 2.52 ± 7.53 6.43 ±.52 OH2.54 ± 3.72.4 ±.78.36 ±.2.4 ±.8 2.8 ± 76.8 7.9 ± 4.66 4.3 ± 2.67 6.8 ± 7.88 4.23 ± 3.6 5.57 ± 4.27 5.6 ± 4.26.9 ± 9.87 OK99.43 ±.6.24 ±.25.26 ±.5.49 ±.8 3.87 ± 5.5 2.76 ± 5.57.47 ± 2.8 2.4 ± 2.66 4.79 ± 3.3 4.2 ± 2.47 2.82 ±.9 5.66 ± 4.9 UT96.59 ±.2.5 ±.23.54 ±.2 22.23 ± 22.98 9.66 ± 3.24 3.6 ± 3.6 4.75 ±.7 3.4 ±.72 29.83 ± 32.72 UT97 2.4 ±.76 2.2 ±.76 2.2 ±.36 2.3 ±.62 8.7 ± 33.89 26.75 ± 36.9 25.9 ± 45.2 9.7 ± 28.38.2 ± 23.6 9. ± 9.63 23.54 ± 92. 2.29 ± 29.4 VT99.63 ±.8.35 ±.26.27 ±.6.63 ±.2 7.2 ± 2.28.6 ± 2.6.32 ± 3. 2.56 ± 2.9 6.98 ± 6.9 3.75 ± 2.8 4.8 ± 4.5 2.37 ± 2.87 WV99.67 ±.2.37 ±.9.64 ±.2 5.2 ±.57 9.86 ± 8.6 2.8 ± 7.42 5.86 ± 8.28 6.98 ± 6.24 8.67 ± 6.22.34 ±.8.23 ±.6.5 ±.4.34 ±.2 3.32 ± 5.2.74 ±.82.5 ±.53.69 ±. 6.55 ± 5.58 3.47 ± 2.44 2.32 ± 2. 8.38 ± 6.49
Figure S. Seasonal average concentrations for (a) GOM (pg m -3 ), (b) PBM (pg m -3 ) and (c) GEM (ng m -3 ). 35 3 25 2 5 5 (a) GOM Spring Summer Fall Winter MD8 MD99 MS2 NH6 NJ5 NJ3 NJ32 NJ54 NS NY6 NY2 NY43 NY95 OH2 OK99 UT96 UT97 VT99 WV99 4 35 (b) PBM 3 25 2 5 5 MD8 MD99 MS2 NH6 NJ5 NJ3 NJ32 NJ54 NS NY6 NY2 NY43 NY95 OH2 OK99 UT96 UT97 VT99 WV99 2.5 2 (c) GEM.5.5 MD8 MD99 MS2 NH6 NJ5 NJ3 NJ32 NJ54 NS NY6 NY2 NY43 NY95 OH2 OK99 UT96 UT97 VT99 WV99
Figure S2. Average diurnal cycle and monthly V d (left columns) and normalized V d by their respective annual average V d (right columns) from 29 data at Kejimkujik forest site. 2.5.3.6 GOM V d ( cm s - ) 2.5.5 2 4 6 8 2468222.25.2.5..5.4.2.8.6.4.2 2 4 6 8 2 4 6 8 2 22.4.2.8.6.4.2 GEM GOM PBM Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec PBM and GEM V d ( cm s - ) Normalized V d 2.5.3 2.5.5.25.2.5..5 Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec Hour Hour GOM V d ( cm s - ) PBM and GEM V d ( cm s - ) Normalized V d