1. Department of Chemistry, University of York, Heslington, York YO10 5DD, UK
2. School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
3. School of Earth and the Environment (SEE), University of Leeds, LS2 9JT, UK
4. Instituto Nacional de Meteorologia Geofísica (INMG), Delegação de São Vicente, Monte, CP 15, Mindelo, Cape Verde
5. National Centre for Atmospheric Science (NCAS), University of York, Heslington, York YO10 5DD, UK
6. Earth and Space Science Division, Jet Propulsion Laboratory, California Institute of Technology, Pasadena, California 91109, USA

Correspondence to: Lucy J. Carpenter¹John M. C. Plane² Correspondence and requests for materials should be addressed to L.J.C. (Email: ljc4@york.ac.uk) or J.M.C.P. (Email: j.m.c.plane@leeds.ac.uk).

Abstract

Increasing tropospheric ozone levels over the past 150 years have led to a significant climate perturbation¹; the prediction of future trends in tropospheric ozone will require a full understanding of both its precursor emissions and its destruction processes. A large proportion of tropospheric ozone loss occurs in the tropical marine boundary layer^{2, 3} and is thought to be driven primarily by high ozone photolysis rates in the presence of high concentrations of water vapour. A further reduction in the tropospheric ozone burden through bromine and iodine emitted from open-ocean marine sources has been postulated by numerical models^{4, 5, 6, 7}, but thus far has not been verified by observations. Here we report eight months of spectroscopic measurements at the Cape Verde Observatory indicative of the ubiquitous daytime presence of bromine monoxide and iodine monoxide in the tropical marine boundary layer. A year-round data set of co-located in situ surface trace gas measurements made in conjunction with low-level aircraft observations shows that the mean daily observed ozone loss is 50 per cent greater than that simulated by a global chemistry model using a classical photochemistry scheme that excludes halogen chemistry. We perform box model calculations that indicate that the observed halogen concentrations induce the extra ozone loss required for the models to match observations. Our results show that halogen chemistry has a significant and extensive influence on photochemical ozone loss in the tropical Atlantic Ocean boundary layer. The omission of halogen sources and their chemistry in atmospheric models may lead to significant errors in calculations of global ozone budgets, tropospheric oxidizing capacity and methane oxidation rates, both historically and in the future.

1. Department of Chemistry, University of York, Heslington, York YO10 5DD, UK
2. School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
3. School of Earth and the Environment (SEE), University of Leeds, LS2 9JT, UK
4. Instituto Nacional de Meteorologia Geofísica (INMG), Delegação de São Vicente, Monte, CP 15, Mindelo, Cape Verde
5. National Centre for Atmospheric Science (NCAS), University of York, Heslington, York YO10 5DD, UK
6. Earth and Space Science Division, Jet Propulsion Laboratory, California Institute of Technology, Pasadena, California 91109, USA

Correspondence to: Lucy J. Carpenter¹John M. C. Plane² Correspondence and requests for materials should be addressed to L.J.C. (Email: ljc4@york.ac.uk) or J.M.C.P. (Email: j.m.c.plane@leeds.ac.uk).

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