Atmos. Chem. Phys. Discuss., 7, 17213-17260, 2007
www.atmos-chem-phys-discuss.net/7/17213/2007/
doi:10.5194/acpd-7-17213-2007
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Seasonal and diurnal variations of Hg° over New England
H. Mao, R. W. Talbot, J. M. Sigler, B. C. Sive, and J. D. Hegarty
Institute for the Study of Earth, Oceans and Space, Climate Change Research Center, University of New Hampshire, Durham, New Hampshire 03824, USA

Abstract. Factors influencing diurnal to interannual variability in Hg° over New England were investigated using multi-year measurements conducted by the AIRMAP program at the Thompson Farm (TF) coastal site, an inland elevated site at Pac Monadnock (PM), and one summer of measurements on Appledore Island (AI) in the Gulf of Maine. Mixing ratios of Hg° at TF showed distinct seasonality with maxima in March and minima in October. In comparison, Hg° at AI tracked the trend at TF but with higher minima, while at PM the diurnal and annual cycles were dampened. In winter, Hg° was correlated most strongly with CO and NOy, indicative of anthropogenic emissions as their primary source. Our analysis indicates that Hg° had a regional background level of ~160 fmol/mol, a summertime dry deposition velocity of ~0.20 cm s−1, and a ~16 day lifetime in the coastal boundary layer. The influence of oceanic emissions on ambient Hg° levels was identified using the Hg°-CHBr3 correlation at both TF and AI. Moreover, the lower Hg° levels and steeper decreasing warm season trend at TF (0.5–0.6 fmol/mol d−1) compared to PM (0.2–0.3 fmol/mol d−1) likely reflected the impact of marine halogen chemistry. Large interannual variability in warm season Hg° levels in 2004 versus 2005/2006 may be due to the role of precipitation patterns in influencing surface evasion of Hg°. In contrast, changes in wintertime maximum levels of Hg° were small compared to drastic reductions in CO, CO2, NOy, and SO2 from 2004/2005 to 2006/2007. These trends could be explained by a homogeneous surface distribution of Hg° over the North American continent in winter and/or rapid removal of mercury released from anthropogenic sources. We caution that during warmer winters, the Hg°-CO slope possibly reflects the ratio of Hg° loss relative to changes in CO more than their emission ratio.

Citation: Mao, H., Talbot, R. W., Sigler, J. M., Sive, B. C., and Hegarty, J. D.: Seasonal and diurnal variations of Hg° over New England, Atmos. Chem. Phys. Discuss., 7, 17213-17260, doi:10.5194/acpd-7-17213-2007, 2007.
 
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