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Modeling the observed tropospheric BrO background: Importance of multiphase chemistry and implications for ozone, OH, and mercury
Open accessAbstract
Aircraft and satellite observations indicate the presence of ppt (ppt ≡ pmol/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 ClNO 3 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 CHBr 3. 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 Bry 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 6 months for elemental mercury. The dominant mechanism for the Br‐Cl driven tropospheric ozone decrease is oxidation of NOx by formation and hydrolysis of BrNO 3 and ClNO 3.
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Cited by
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Young, P. J., Naik, V., Fiore, A. M., Gaudel, A., Guo, J., Lin, M. Y., Neu, J. L., Parrish, D. D., Rieder, H. E., Schnell, J. L., et al. (2018) · Elementa: Science of the Anthropocene · doi:10.1525/elementa.265 · Cited by 444
Self-citationGlobal impacts of tropospheric halogens (Cl, Br, I) on oxidants and composition in GEOS-Chem
Sherwen, T., Schmidt, J. A., Evans, M. J., Carpenter, L. J., Großmann, K., Eastham, S. D., Jacob, D. J., Dix, B., Koenig, T. K., Sinreich, R., et al. (2016) · Atmospheric Chemistry and Physics · doi:10.5194/acp-16-12239-2016 · Cited by 375
Self-citationTropospheric Ozone Assessment Report
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Self-citationHu, L., Jacob, D. J., Liu, X., Zhang, Y., Zhang, L., Kim, P. S., Sulprizio, M. P., & Yantosca, R. M. (2017) · Atmospheric Environment · doi:10.1016/j.atmosenv.2017.08.036 · Cited by 148
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Metadata
- Authors
- 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., & Volkamer, R.
- Venue
- Journal of Geophysical Research: Atmospheres
- Publisher
- American Geophysical Union (AGU)
- Published
- 2016-10
- Volume
- 121
- Issue
- 19
- ISSN
- 0148-0227 (ISSN-L)
- 2169-897X
- 2169-8996
- OpenAlex
- W2518980494
- Cited by
- 176
- References
- 0
- FWCI
- 13.08
- Type
- journal article
- Language
- en
- Open access
- green
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- 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., & 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. https://doi.org/10.1002/2015jd024229
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