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A global model study of natural bromine sources and the effects on tropospheric chemistry using MOZART4

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Abstract

Halogens in the atmosphere chemically destroy ozone. In the troposphere, bromine has higher ozone destruction efficiency than chlorine and is the halogen species with the widest geographical spread of natural sources. We investigate the relative strength of various sources of reactive tropospheric bromine and the influence of bromine on tropospheric chemistry using a 6-year simulation with the global chemistry transport model MOZART4. We consider the following sources: short-lived bromocarbons (CHBr3, CH2BrCl, CHBr2Cl, CHBrCl2, and CH2Br2) and CH3Br, bromine from airborne sea salt particles, and frost flowers and sea salt on or in the snowpack in polar regions. The total bromine emissions in our simulations add up to 31.7 Gmol(Br)/yr: 63 % from polar sources, 24.6 % from short-lived bromocarbons and 12.4 % from airborne sea salt particles. We conclude from our analysis that our global bromine emission is likely to be on the lower end of the range, because of too low emissions from airborne sea salt. Bromine chemistry has an effect on the oxidation capacity of the troposphere, not only due to its direct influence on ozone concentrations, but also by reactions with other key chemical species like HO x and NO x . Globally, the impact of bromine chemistry on tropospheric O3 is comparable to the impact of gas-phase sulfur chemistry, since the inclusion of bromine chemistry in MOZART4 leads to a decrease of the O3 burden in the troposphere by 6 Tg, while we get an increase by 5 Tg if gas-phase sulfur chemistry is switched off in the standard model. With decreased ozone burden, the simulated oxidizing capacity of the atmosphere decreases thus affecting species associated with the oxidation capacity of the atmosphere (CH3OOH, H2O2).

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Notes

  1. Very-short lived species are species with lifetimes lower than half an year according to definition of the World Meteorological Organization (2010).

  2. For simplicity, we use a tropopause at 100 hPa throughout our study.

  3. Products from the Satellite GOME can be visualized at http://www.doas-bremen.de/bro_from_gome.htm. Last accessed February 5, 2011.

  4. See http://arctic.atmos.uiuc.edu/cryosphere/. Last accessed February 17, 2011.

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Acknowledgements

GSS and SR are very grateful to Guy Brasseur for interesting and enlightening discussions. The authors further thank Louisa Emmons, Jean-François Lamarque, John Orlando, and Stacy Walters (in alphabetical order) for their advice in many aspects of the usage of MOZART4 and their fruitful discussion about the model setup. The authors also thank Andreas Richter and Lars Kaleschke for sharing their expertise in satellite retrievals and sea salt chemistry and physics. The authors are grateful to the reviewers who helped to improve this contribution considerably.

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  1. Institute for Atmospheric and Climate Science, ETHZ, Zurich, Switzerland

    Gabriela Sousa Santos

  2. Max Planck Institut for Meteorology, Hamburg, Germany

    Sebastian Rast

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  1. Gabriela Sousa Santos
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  2. Sebastian Rast
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Correspondence to Gabriela Sousa Santos.

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Sousa Santos, G., Rast, S. A global model study of natural bromine sources and the effects on tropospheric chemistry using MOZART4. J Atmos Chem 70, 69–89 (2013). https://doi.org/10.1007/s10874-013-9252-y

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  • DOI: https://doi.org/10.1007/s10874-013-9252-y

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