Atmos. Chem. Phys. Discuss., 13, 3575-3611, 2013
© Author(s) 2013. This work is distributed
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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.
Cloud-resolving simulations of mercury scavenging and deposition in thunderstorms
U. S. Nair1, Y. Wu2, C. D. Holmes3, A. Ter Schure4, G. Kallos5, and J. T. Walters6
1Department of Atmospheric Science, University of Alabama in Huntsville, 320 Sparkman Drive, Alabama 35805, USA
2Earth System Science Center, University of Alabama in Huntsville, 320 Sparkman Drive, Huntsville, Alabama 35805, USA
3Department of Earth System Science, University of California, Irvine, California 92697, USA
4Electric Power Research Institute, Palo Alto, CA 94304, USA
5School of Physics, University of Athens, Athens, Greece
6Southern Company Services, Birmingham, AL 35203, USA

Abstract. This study examines dynamical and microphysical features of convective clouds that affect mercury (Hg) wet scavenging and concentrations in rainfall. Using idealized numerical model simulations in the Regional Atmospheric Modeling System (RAMS), we diagnose vertical transport and scavenging of soluble Hg species in thunderstorms under typical environmental conditions found in the Northeast and Southeast United States (US). Three important environmental characteristics that impact thunderstorm morphology were studied: convective available potential energy (CAPE), vertical shear (0–6 km) of horizontal wind (SHEAR) and precipitable water (PW).

We find that in a strong convective storm in the Southeast US that about 40% of mercury in the boundary layer (0–2 km) can be scavenged and deposited to the surface. Removal efficiencies are 35% or less in the free troposphere and decline with altitude. Nevertheless, if we assume that soluble Hg species are initially uniformly mixed vertically, then about 60% deposited mercury deposited by the thunderstorm originates in the free troposphere.

For a given CAPE, storm morphology and Hg deposition respond to SHEAR and PW. Experiments show that the response of mercury concentration in rainfall to SHEAR depends on the amount of PW. For low PW, increasing SHEAR decreases mercury concentrations in high-rain amounts (>13 mm). However, at higher PW values, increasing SHEAR decreases mercury concentrations for all rainfall amounts. These experiments suggest that variations in environmental characteristics relevant to thunderstorm formation and evolution can also contribute to geographical difference in wet deposition of mercury.

An ensemble of thunderstorm simulations was also conducted for different combinations of CAPE, SHEAR and PW values derived from radiosonde observations at five sites in the Northeast United States (US) and at three sites in the Southeast US. Using identical initial concentrations of gaseous oxidized mercury (GOM) and particle-bound mercury (HgP), from the GEOS-Chem model, the simulations predict higher mercury concentrations in rainfall from thunderstorms forming in the environmental conditions over the Southeast US compared to the Northeast US.

Mercury concentrations in rainfall are also simulated for a typical stratiform rain event and found to be less than in thunderstorms forming in environments typical of the Southeast US. The stratiform cloud scavenges mercury from the lower ~4 km of the atmosphere, while thunderstorms scavenge up to ~10 km.

Citation: Nair, U. S., Wu, Y., Holmes, C. D., Ter Schure, A., Kallos, G., and Walters, J. T.: Cloud-resolving simulations of mercury scavenging and deposition in thunderstorms, Atmos. Chem. Phys. Discuss., 13, 3575-3611, doi:10.5194/acpd-13-3575-2013, 2013.
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