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dc.contributor.authorAmos, Helen Marie
dc.contributor.authorJacob, Daniel J.
dc.contributor.authorHolmes, C. D.
dc.contributor.authorFisher, Jenny Allison
dc.contributor.authorWang, Qiaoqiao
dc.contributor.authorYantosca, Robert M.
dc.contributor.authorCorbitt, Elizabeth Sturges
dc.contributor.authorGalarneau, E.
dc.contributor.authorRutter, A. P.
dc.contributor.authorGustin, M. S.
dc.contributor.authorSteffen, A.
dc.contributor.authorSchauer, J. J.
dc.contributor.authorGraydon, J. A.
dc.contributor.authorLouis, V. L. St.
dc.contributor.authorTalbot, R. W.
dc.contributor.authorEdgerton, E. S.
dc.contributor.authorZhang, Y.
dc.contributor.authorSunderland, Elynor M
dc.date.accessioned2014-03-14T13:10:59Z
dc.date.issued2012
dc.identifier.citationAmos, H. M., D. J. Jacob, C. D. Holmes, J. A. Fisher, Q. Wang, R. M. Yantosca, E. S. Corbitt, et al. 2012. Gas-Particle Partitioning of Atmospheric Hg(II) and Its Effect on Global Mercury Deposition. Atmospheric Chemistry and Physics 12, no. 1: 591–603.en_US
dc.identifier.issn1680-7316en_US
dc.identifier.issn1680-7324en_US
dc.identifier.urihttp://nrs.harvard.edu/urn-3:HUL.InstRepos:11891561
dc.description.abstractAtmospheric deposition of Hg(II) represents a major input of mercury to surface environments. The phase of Hg(II) (gas or particle) has important implications for deposition. We use long-term observations of reactive gaseous mercury (RGM, the gaseous component of Hg(II)), particle-bound mercury (PBM, the particulate component of Hg(II)), fine particulate matter (PM2.5), and temperature (T) at five sites in North America to derive an empirical gas-particle partitioning relationship log10(K−1) = (10±1)–(2500±300)/T where K = (PBM/PM2.5)/RGM with PBM and RGM in common mixing ratio units, PM2.5 in μg m−3, and T in K. This relationship is within the range of previous work but is based on far more extensive data from multiple sites. We implement this empirical relationship in the GEOS-Chem global 3-D Hg model to partition Hg(II) between the gas and particle phases. The resulting gas-phase fraction of Hg(II) ranges from over 90 % in warm air with little aerosol to less than 10 % in cold air with high aerosol. Hg deposition to high latitudes increases because of more efficient scavenging of particulate Hg(II) by precipitating snow. Model comparison to Hg observations at the North American surface sites suggests that subsidence from the free troposphere (warm air, low aerosol) is a major factor driving the seasonality of RGM, while elevated PBM is mostly associated with high aerosol loads. Simulation of RGM and PBM at these sites is improved by including fast in-plume reduction of Hg(II) emitted from coal combustion and by assuming that anthropogenic particulate Hg(p) behaves as semi-volatile Hg(II) rather than as a refractory particulate component. We improve the simulation of Hg wet deposition fluxes in the US relative to a previous version of GEOS-Chem; this largely reflects independent improvement of the washout algorithm. The observed wintertime minimum in wet deposition fluxes is attributed to inefficient snow scavenging of gas-phase Hg(II).en_US
dc.description.sponsorshipEarth and Planetary Sciencesen_US
dc.description.sponsorshipEngineering and Applied Sciencesen_US
dc.language.isoen_USen_US
dc.publisherCopernicus GmbHen_US
dc.relation.isversionofdoi:10.5194/acp-12-591-2012en_US
dash.licenseLAA
dc.titleGas-Particle Partitioning of Atmospheric Hg(II) and Its Effect on Global Mercury Depositionen_US
dc.typeJournal Articleen_US
dc.description.versionVersion of Recorden_US
dc.relation.journalAtmospheric Chemistry and Physicsen_US
dash.depositing.authorJacob, Daniel J.
dc.date.available2014-03-14T13:10:59Z
dash.affiliation.otherDepartment of Environmental Health, School of Public Healthen_US
dc.identifier.doi10.5194/acp-12-591-2012*
workflow.legacycommentscan post pub per sherpa. FAR 2013en_US
dash.authorsorderedfalse
dash.contributor.affiliatedAmos, Helen
dash.contributor.affiliatedCorbitt, Elizabeth Sturges
dash.contributor.affiliatedFisher, Jenny
dash.contributor.affiliatedWang, Qiaoqiao
dash.contributor.affiliatedSunderland, Elynor
dash.contributor.affiliatedYantosca, Robert
dash.contributor.affiliatedJacob, Daniel


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