Halogens released from long-lived anthropogenic substances, such as chlorofluorocarbons, are the principal cause of recent depletion of stratospheric ozone, a greenhouse gas1,2,3. Recent observations show that very short-lived substances, with lifetimes generally under six months, are also an important source of stratospheric halogens4,5. Short-lived bromine substances are produced naturally by seaweed and phytoplankton, whereas short-lived chlorine substances are primarily anthropogenic. Here we used a chemical transport model to quantify the depletion of ozone in the lower stratosphere from short-lived halogen substances, and a radiative transfer model to quantify the radiative effects of that ozone depletion. According to our simulations, ozone loss from short-lived substances had a radiative effect nearly half that from long-lived halocarbons in 2011 and, since pre-industrial times, has contributed a total of about −0.02 W m−2 to global radiative forcing. We find natural short-lived bromine substances exert a 3.6 times larger ozone radiative effect than long-lived halocarbons, normalized by halogen content, and show atmospheric levels of dichloromethane, a short-lived chlorine substance not controlled by the Montreal Protocol, are rapidly increasing. We conclude that potential further significant increases in the atmospheric abundance of short-lived halogen substances, through changing natural processes6,7,8 or continued anthropogenic emissions9, could be important for future climate.
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Myhre, G. et al. in Climate Change 2013: The Physical Science Basis (eds Stocker, T. F. et al.) Ch. 8, 659–740 (IPCC, Cambridge Univ. Press, 2013).
Riese, M. et al. Impact of uncertainties in atmospheric mixing on simulated UTLS composition and related radiative effects. J. Geophys. Res. 117, D16305 (2012).
Montzka, S. A. & Reimann, S. Scientific Assessment of Ozone Depletion: 2010, Global Ozone Research and Monitoring Project Report No. 52, Ch. 1 (World Meteorological Organization, 2011).
Sturges, W. T., Oram, D. E., Carpenter, L. J., Penkett, S. A. & Engel, A. Bromoform as a source of stratospheric bromine. Geophys. Res. Lett. 27, 2081–2084 (2000).
Laube, J. C. et al. Contribution of very short-lived organic substances to stratospheric chlorine and bromine in the tropics—a case study. Atmos. Chem. Phys. 8, 7325–7334 (2008).
Dessens, O., Zeng, G., Warwick, N. & Pyle, J. Short-lived bromine compounds in the lower stratosphere; impact of climate change on ozone. Atmos. Sci. Lett. 10, 201–206 (2009).
Hossaini, R. et al. Modelling future changes to the stratospheric source gas injection of biogenic bromocarbons. Geophys. Res. Lett. 39, L20813 (2012).
Hepach, H. et al. Drivers of diel and regional variations of halocarbon emissions from the tropical North East Atlantic. Atmos. Chem. Phys. 14, 1255–1275 (2014).
Leedham, E. C. et al. Emission of atmospherically significant halocarbons by naturally occurring and farmed tropical macroalgae. Biogeosciences 10, 3615–3633 (2013).
Dorf, M. et al. Bromine in the tropical troposphere and stratosphere as derived from balloon-borne BrO observations. Atmos. Chem. Phys. 8, 7265–7271 (2008).
Hossaini, R. et al. Evaluating global emission inventories of biogenic bromocarbons. Atmos. Chem. Phys. 13, 11819–11838 (2013).
Aschmann, J., Sinnhuber, B. M., Chipperfield, M. P. & Hossaini, R. Impact of deep convection and dehydration on bromine loading in the upper troposphere and lower stratosphere. Atmos. Chem. Phys. 11, 2671–2687 (2011).
Salawitch, R. J. et al. Sensitivity of ozone to bromine in the lower stratosphere. Geophys. Res. Lett. 32, L05811 (2005).
Feng, W., Chipperfield, M. P., Dorf, M., Pfeilsticker, K. & Ricaud, P. Mid-latitude ozone changes: Studies with a 3-D CTM forced by ERA-40 analyses. Atmos. Chem. Phys. 7, 2357–2369 (2007).
Sinnhuber, B. M., Sheode, N., Sinnhuber, M., Chipperfield, M. P. & Feng, W. The contribution of anthropogenic bromine emissions to past stratospheric ozone trends: A modelling study. Atmos. Chem. Phys. 9, 2863–2871 (2009).
Chipperfield, M. P. New version of the TOMCAT/SLIMCAT off-line chemical transport model: Intercomparison of stratospheric tracer experiments. Q. J. R. Meteorol. Soc. 132, 1179–1203 (2006).
Edwards, J. M. & Slingo, A. Studies with a flexible new radiation code. 1. Choosing a configuration for a large-scale model. Q. J. R. Meteorol. Soc. 122, 689–719 (1996).
Rap, A. et al. Natural aerosol direct and indirect radiative effects. Geophys. Res. Lett. 40, 3297–3301 (2013).
Simmonds, P. G. et al. Global trends, seasonal cycles, and European emissions of dichloromethane, trichloroethene, and tetrachloroethene from the AGAGE observations at Mace Head, Ireland, and Cape Grim, Tasmania. J. Geophys. Res. 111, D18304 (2006).
Worton, D. R. et al. 20th century trends and budget implications of chloroform and related tri-and dihalomethanes inferred from firn air. Atmos. Chem. Phys. 6, 2847–2863 (2006).
Bosch, H. et al. Upper limits of stratospheric IO and OIO inferred from center-to-limb-darkening-corrected balloon-borne solar occultation visible spectra: Implications for total gaseous iodine and stratospheric ozone. J. Geophys. Res. 108, 4455 (2003).
Carpenter, L. J. et al. Atmospheric iodine levels influenced by sea surface emissions of inorganic iodine. Nature Geosci. 6, 108–111 (2013).
Saiz-Lopez, A. et al. Estimating the climate significance of halogen-driven ozone loss in the tropical marine troposphere. Atmos. Chem. Phys. 12, 3939–3949 (2012).
Dix, B. et al. Detection of iodine monoxide in the tropical free troposphere. Proc. Natl Acad. Sci. USA 110, 2035–2040 (2013).
Rasch, P. J. et al. An overview of geoengineering of climate using stratospheric sulphate aerosols. Phil. Trans. R. Soc. A 366, 4007–4037 (2008).
Campbell, N. et al. in Safeguarding the Ozone Layer and the Global Climate System: Issues Related to Hydrofluorocarbons and Perfluorocarbons (eds Metz, B. et al.) Ch. 11, 403–436 (IPCC/TEAP, Cambridge Univ. Press, 2005).
Velders, G. J. M., Fahey, D. W., Daniel, J. S., McFarland, M. & Andersen, S. O. The large contribution of projected HFC emissions to future climate forcing. Proc. Natl Acad. Sci. USA 106, 10949–10954 (2009).
Laube, J. C. et al. Newly detected ozone-depleting substances in the atmosphere. Nature Geosci. 7, 266–269 (2014).
Saltzman, E. S., Aydin, M., Williams, M. B., Verhulst, K. R. & Gun, B. Methyl chloride in a deep ice core from Siple Dome, Antarctica. Geophys. Res. Lett. 36, L03822 (2009).
Montzka, S. A. et al. Small interannual variability of global atmospheric hydroxyl. Science 331, 67–69 (2011).
We thank NERC for funding (TropHal project, NE/J02449X/1). Ground-based observations of CH2Cl2 are supported in part by NOAA’s Climate Program Office through its Atmospheric, Chemistry, Carbon Cycle and Climate Program. C. Siso, B. Hall, J. Elkins and B. Miller provided assistance in making and standardizing these measurements.
The authors declare no competing financial interests.
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Hossaini, R., Chipperfield, M., Montzka, S. et al. Efficiency of short-lived halogens at influencing climate through depletion of stratospheric ozone. Nature Geosci 8, 186–190 (2015). https://doi.org/10.1038/ngeo2363
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