ACPD Atmospheric Chemistry and Physics Discussions ACPD 1680-7375 Copernicus GmbH Göttingen, Germany 10.5194/acpd-9-8737-2009 Oceanic influence on atmospheric mercury at coastal and inland sites: a springtime noreaster in New England Sigler J. M. 1 Mao H. 1 Sive B. C. 1 Talbot R. 1 Institute for the Study of Earth, Oceans and Space, Climate Change Research Center, University of New Hampshire, Morse Hall, 8 College Road, Durham, NH 03824-3525, USA 01 04 2009 9 2 8737 8755 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys-discuss.net/9/8737/2009/acpd-9-8737-2009.html The full text article is available as a PDF file from http://www.atmos-chem-phys-discuss.net/9/8737/2009/acpd-9-8737-2009.pdf

Continuous measurements of elemental (Hg<sup>0</sup>) and reactive mercury were conducted at two sites in New Hampshire during a powerful April 2007 noreaster. During the most intense period of the storm, enhancements of ~30–50 ppqv in Hg<sup>0</sup> were observed at a coastal and a high elevation inland site. This enhancement occurred simultaneously with elevated mixing ratios of three marine tracers, CH<sub>3</sub>I, CH<sub>2</sub>Br<sub>2</sub> and CHBr<sub>3</sub>. These observations suggest a marine source of Hg<sup>0</sup>, possibly outgassing from the ocean surface during strong turbulence. The Hg<sup>0</sup> enhancement observed 100 km inland suggests that the impact of coastal storms on terrestrial Hg cycling may not be limited to near-shore environments. Combining Hg<sup>0</sup> and marine tracer measurements during the storm with estimates of oceanic tracer fluxes during previous strong storms yields an order-of-magnitude estimate of the oceanic source of Hg<sup>0</sup> during the storm (~7 ppqv hr<suP&minus1;</sup>) which can account for the observed enhancement at the field sites.

 References Andersson, M., G&aring;rdfeldt, K., Wängberg, I., Sprovieri, F., Pirrone, N., and Lindqvist, O.: Seasonal and daily variation of mercury evasion at coastal and off shore sites from the Mediterranean Sea, Marine Chem., 104, 214–216, 2007. Bash, J O. and Miller, D R.: A~relaxed eddy accumulation system for measuring surface fluxes of total gaseous mercury, J. Atmos. Oceanic Tech., 25, 244–257, 2008. Blake, N J., Blake, D R., Simpson, I J., Lopez, J P., Johnston, N A C., Swanson, A L., Katzenstein, A S., Meinardi, S., Sive, B C., Colman, J J., Atlas, E., Flocke, F., Vay, S A., Avery, M A., and Rowland, F S.: Large-scale latitudinal and vertical distributions of NMHCs and selected halocarbons in the troposphere over the Pacific Ocean during the March–April 1999 Pacific Exploratory Mission (PEM-Tropics B), J. Geophys. Res., 106(D23), 32627–32644, 2001. Butler, J H., King, D B., Lobert, J M., Montzka, S A., Yvon-Lewis, S A., Hall, B D., Warwick, N J., Mondeel, D J., Aydin, M., and Elkins, J W.: Oceanic distributions and emissions of short-lived halocarbons, Global Biogeochem. Cy., 21, GB1023, doi:10.1029/2006GB002732, 2007. Carpenter, L. J., Liss, P. S., and Penkett, S A.: Marine organohalogens in the atmosphere over the Atlantic and Southern Oceans, J. Geophys. Res., 108, 4256, doi:10.1029/2002JD002769, 2003. Draxler, R R. and Rolph, G D.: HYSPLIT (HYbrid Single-Particle Lagrangian Integrated Trajectory) Model access via http://www.arl.noaa.gov/ready/hysplit4.html, NOAA Air Resources Laboratory, Silver Spring, MD, 2003. Ebinghaus, R., Kock, H H., Coggins, A M., Spain, T G., Jennings, S G., and Temme, C.: Long-term measurements of atmospheric mercury concentrations at Mace Head, Irish west coast, between 1995 and 2001, Atmos. Environ., 36, 5267–5276, 2002. Engle, M A., Tate, M T., Krabbenhoft, D P., Kolker, A., Olson, M L., Edgerton, E S., DeWild, J F., and McPherson, A K.: Characterization and cycling of atmospheric mercury along the central US Gulf Coast, Appl. Geochem., 23, 419–437, 2008. Ferrara, R., Mazzolai, B., Lanzillotta, E., Nucaro, E., and Pirrone, N.: Temporal trends in gaseous mercury evasion from the Mediterranean seawaters, Sci. Total Env., 259, 183–190, 2000. G&aring;rdfeldt, K., Sommar, J., Ferrara, R., Ceccarini, C., Lanzillotta, E., Munthe, J., Wängberg, I., Lindqvist, O., Pirrone, N., Sprovieri, F., Pesenti, E., and Strömberg, D.: Evasion of mercury from coastal and open waters of the Atlantic Ocean and the Mediterranean Sea, Atmos. Env., 37(S1), S73–S84, 2003. Guentzel, J L., Landing, W M., Gill, G A., and Pollman, C D.: Processes influencing rainfall deposition of mercury in Florida, Environ. Sci. Tech., 35, 863–873, 2001. Gustin, M S. and Stamenkovic, L.: Effect of watering and soil moisture on mercury emissions from soils, Biogeochemistry, 76, 215–232, 2005. Hedgecock, I M. and Pirrone, N.: Chasing quicksilver: Modeling the atmospheric lifetime of \chemHg^0(g) in the marine boundary layer at various latitudes, Environ. Sci. Technol., 38, 69–76, 2004. Hedgecock, I M., Trunfio, G A., Pirrone, N., and Sprovieri, F.: Mercury chemistry in the MBL: Mediterranean case and sensitivity studies using the AMCOTS (Atmospheric Mercury Chemistry over the Sea) model, Atmos. Environ., 39, 7217–7230, 2005. Kock, H H., Beiber, E., Ebinghaus, R., Spain, T G., and Thees, B.: Comparison of long-term trends and seasonal variations of atmospheric mercury concentrations at the two European coastal monitoring stations Mace Head, Ireland and Zingst, Germany, Atmos. Environ., 39, 7549–7556, 2005. Kuss, J. and Schneider, B.: Variability of the gaseous elemental mercury sea-air flux of the Baltic Sea, Environ. Sci. Technol., 41, 8018–8023, 2007. Lamborg, C H., Fitzgerald, W F., O'Donnell, J., and Torgeson, T.: A~non-steady state compartmental model of global-scale mercury biogeochemistry with interhemispheric atmospheric gradients, Geochim. Cosmochim. Ac., 66, 1105–1118, 2002. Laurier, F.J.G., Mason, R. P., Whalin, L., and Kato, S.: Reactive gaseous mercury formation in the North Pacific Ocean's marine boundary layer: A~potential role of halogen chemistry, J. Geophys. Res., 108(D17), 4529, doi:10.1029/2003JD003625, 2003. Laurier, F. and Mason, R.: Mercury concentration and speciation in the coastal and open ocean boundary layer, J. Geophys. Res., 112, D06302, doi:10.1029/2006JD007320, 2007. Lindberg, S E., Zhang, H., Gustin, M., Vette, A., Marsik, F., Owens, J., Casimir, A., Ebinghaus, R., Edwards, G., Fitzgerald, C., Kemp, J., Kock, H H., London, J., Majewski, M., Poissant, L., Pilote, M., Rasmussen, P., Schaedlich, F., Schneeberger, D., Sommar, J., Turner, R., Wallschläger, D., and Xiao, Z.: Increases in mercury emission from desert soils in response to rainfall and irrigation, J Geophys. Res., 104(D17), 21879–888, 1999. Malcolm, E G., Keeler, G J., and Landis, M S.: The effects of the coastal environment on the atmospheric mercury cycle, J. Geophys. Res., 108, doi:10.1029/2002JD003084, 2003. Mao, H. and Talbot, R.: \chemO_3 and \chemCO in New England: Temporal variation and relationships, J. Geophys. Res., 109, D21304, doi:10.1029/2004JD004913, 2004. Mao, H., Talbot, R., Sigler, J M., Sive, B C., and Hegarty, J.: Seasonal and diurnal variation of \chemHg^0 over New England, Atmos. Chem. Phys., 8, 1403–1421, 2008. Mason, R P., Rohlfus, K R., and Fitzgerald, W F.: Mercury in the North Atlantic, Mar. Chem., 61, 37–53, 1998. Mason, R P., Lawson, N M., and Sheu, G.-R.: Mercury in the Atlantic Ocean: factors controlling air-sea exchange of mercury and its distribution in the upper waters, Deep-Sea Res. II, 48, 2829–2853, 2001. Mason, R P. and Sheu, G.-R.: Role of the ocean in the global mercury cycle, Global Biogeochem. Cy., 16(4), 1093, doi:10.1029/2001GB001440, 2002. Pirrone, N., Ferrara, R., Hedgecock, I M., Kallos, G., Mamane, Y., Munthe, J., Pacyna, J M., Pytharoulis, I., Sprovieri, F., Voudouri, A., and Wangberg, I.: Dynamic processes of mercury over the Mediterranean region: Results from the Mediterranean Atmospheric Mercury Cycle System (MAMCS) project, Atmos. Env., 37(S1), S21–S39, 2003 Rolfhus, K R. and Fitzgerald, W F.: Mechanisms and temporal variability of dissolved gaseous mercury production in coastal seawater, Marine Chem., 90, 125–136, 2004. Sigler, J M., Mao, H., and Talbot, R.: Gaseous elemental and reactive mercury in southern New Hampshire, Atmos. Chem. Phys., 9, 1929–1942, 2009. Sillman, S., Marsik, F J., Al-Wali, K I., Keeler, G J., and Landis, M S.: Reactive mercury in the troposphere: Model formation and results for Florida, the northeastern United States, and the Atlantic Ocean, J Geophys. Res., 112, D23305, doi:10.1029/2006JD008227, 2007. Sive, B C., Varner, R K., Mao, H., Blake, D R., Wingenter, O W., and Talbot, R.: A~large terrestrial source of methyl iodide, J. Geophys. Res. 34, L17808, doi:10.1029/2007GL030528, 2007. Sprovieri, F., Pirrone, N., G&aring;rdfeldt, K., and Sommar, J.: Mercury speciation in the marine boundary layer along a~6000 km cruise path around the Mediterranean Sea, Atmos. Env., 37(S1), S63–S71, 2003. Strode, S A., Jaegle, L., Selin, N E., Jacob, D J., Park, R J., Yantosca, R M., Mason, R.P., and Slemr, F.: Air-sea exchange in the global mercury cycle, Global Biogeochem. Cy., 21, GB1017, doi:10.1029/2006GB002766, 2007. Wanninkhof, R.: Relationship between wind speed and gas exchange over the ocean, J. Geophys. Res., 97, 7373–7382, 1992. Zhou, Y., Varner, R K., Russo, R S., Wingenter, O W., Haase, K B., Talbot, R., and Sive, B C.: Coastal water source of short-lived halocarbons in New England, J. Geophys. Res., 110, D21302, doi:10.1029/2004JD005603, 2005. Zhou, Y., Mao, H., Russo, R. S., Blake, D. R., Wingenter, O. W., Haase, K. B., Ambrose, J., Varner, R. K., Talbot, R., and Sive, B. C.: Bromoform and dibromomethane measurements in the seacoast region of New Hampshire, 2002–2004, J. Geophys. Res., 113, D08305, doi:10.1029/2007JD009103, 2008.