Modeling the observed tropospheric BrO background: Importance of multiphase chemistry and implications for ozone, OH, and mercury

Schmidt, J. A., Jacob, D. J., Horowitz, H. M., Hu, L., Sherwen, T., Evans, M. J., Liang, Q., Suleiman, R. M., Oram, D. E., Le Breton, M., Percival, C. J., Wang, S., Dix, B. and Volkamer, R. (2016) Modeling the observed tropospheric BrO background: Importance of multiphase chemistry and implications for ozone, OH, and mercury. Journal of Geophysical Research: Atmospheres, 121 (19). pp. 11819-11835. ISSN 2169-897X

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Abstract

Aircraft and satellite observations indicate the presence of ppt (pptpmol/mol) levels of BrO in the free troposphere with important implications for the tropospheric budgets of ozone, OH, and mercury. We can reproduce these observations with the GEOS-Chem global tropospheric chemistry model by including a broader consideration of multiphase halogen (Br-Cl) chemistry than has been done in the past. Important reactions for regenerating BrO from its nonradical reservoirs include HOBr+Br-/Cl- in both aerosols and clouds, and oxidation of Br- by ClNO3 and ozone. Most tropospheric BrO in the model is in the free troposphere, consistent with observations and originates mainly from the photolysis and oxidation of ocean-emitted CHBr3. Stratospheric input is also important in the upper troposphere. Including production of gas phase inorganic bromine from debromination of acidified sea salt aerosol increases free tropospheric Br-y by about 30%. We find HOBr to be the dominant gas-phase reservoir of inorganic bromine. Halogen (Br-Cl) radical chemistry as implemented here in GEOS-Chem drives 14% and 11% decreases in the global burdens of tropospheric ozone and OH, respectively, a 16% increase in the atmospheric lifetime of methane, and an atmospheric lifetime of 6months for elemental mercury. The dominant mechanism for the Br-Cl driven tropospheric ozone decrease is oxidation of NOx by formation and hydrolysis of BrNO3 and ClNO3.

Item Type:	Article
Uncontrolled Keywords:	halogen,troposphere,ozone,mercury,modeling,geos-chem,marine boundary-layer,sea-salt aerosols,bromine chemistry,global observations,halogen chemistry,iodine chemistry,north-atlantic,geos-chem,in-situ,constraints,sdg 14 - life below water ,/dk/atira/pure/sustainabledevelopmentgoals/life_below_water
Faculty \ School:	Faculty of Science > School of Environmental Sciences
UEA Research Groups:	Faculty of Science > Research Groups > Atmospheric Chemistry (former - to 2018) Faculty of Science > Research Groups > Climate, Ocean and Atmospheric Sciences (former - to 2017) Faculty of Science > Research Groups > Centre for Ocean and Atmospheric Sciences
Depositing User:	Pure Connector
Date Deposited:	23 Dec 2016 00:01
Last Modified:	07 Oct 2023 00:53
URI:	https://ueaeprints.uea.ac.uk/id/eprint/61882
DOI:	10.1002/2015JD024229

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