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Preprints
https://doi.org/10.5194/acp-2019-1091
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2019-1091
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 24 Jan 2020

Submitted as: research article | 24 Jan 2020

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A revised version of this preprint was accepted for the journal ACP and is expected to appear here in due course.

Seasonal impact of biogenic VSL bromine on the evolution of mid-latitude lowermost stratospheric ozone during the 21st century

Javer A. Barrera1, Rafael P. Fernandez1,2,3, Fernando Iglesias-Suarez2, Carlos A. Cuevas2, Jean-Francois Lamarque4, and Alfonso Saiz-Lopez2 Javer A. Barrera et al.
  • 1Institute for Interdisciplinary Science, National Research Council (ICB-CONICET), FCEN-UNCuyo, Mendoza, 5500, Argentina
  • 2Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, CSIC, Madrid, 28006, Spain
  • 3Atmospheric and Environmental Studies Group (GEAA), UTN-FRM, Mendoza, 5500, Argentina
  • 4Atmospheric Chemistry, Observations & Modelling Laboratory, National Center for Atmospheric Research, Boulder, CO 80301, USA

Abstract. Biogenic very short-lived bromine (VSLBr) represents, nowadays, ~ 25 % of the total stratospheric bromine loading. Owing to their much shorter lifetime compared to anthropogenic long-lived bromine (LLBr, e.g., halons) and chlorine (LLCl, e.g., chlorofluorocarbons) substances, the impact of VSLBr on ozone peaks at the extratropical lowermost stratosphere, a key climatic and radiative atmospheric region. Here we present a modelling study of the evolution of stratospheric ozone and its chemical losses in extra-polar regions during the 21st century, under two different scenarios: considering and neglecting the additional stratospheric injection of 5 ppt biogenic VSLBr naturally released from the ocean. Our analysis shows that the inclusion of VSLBr result in a realistic stratospheric bromine loading and improves the quantitative 1980–2015 model-satellite agreement of total ozone column (TOC) in the mid-latitudes. We show that the overall ozone response to VSLBr within the mid-latitudes follows the stratospheric abundances evolution of long-lived inorganic chlorine and bromine throughout the 21st century. Additional ozone losses due to VSLBr are maximised during the present-day period (1990–2010), with TOC differences of −8 DU (−3 %) and −5.5 DU (−2 %) for the southern (SH-ML) and northern (NH-ML) mid-latitudes, respectively. Moreover, the projected TOC differences at the end of the 21st century are at least half of the values found for the present-day period. In the tropics, a small (< −2.5 DU) and relatively constant (~ −1 %) ozone depletion mediated by VSL-bromine is closely related to its fixed emissions throughout the modelling period. We find that the seasonal VSLBr impacts on mid-latitude lowermost stratospheric ozone are influenced by the seasonality of the inorganic chlorine heterogeneous reactivation processes on ice-crystals. Indeed, due to the more efficient reactivation of chlorine reservoirs (mainly ClONO2 and HCl) within the colder SH-ML lowermost stratosphere, the seasonal VSLBr impact shows a small but persistent hemispheric asymmetry through the whole modelling period. The largest modelled VSLBr impacts occur during the spring with local ozone changes during the present-day period of up to −10 % and −7 % at SH-ML and NH-ML, respectively. Our results indicate that, although the overall VSLBr-driven ozone destruction is largest during the spring, the halogen-mediated ozone depletion (Halog–Loss) in the mid-latitude lowermost stratosphere (~120 hPa) during the winter is comparatively more efficient than the HOx catalytic cycles respect to other seasons. Indeed, when VSLBr are considered, Halog–Loss dominates wintertime SH-ML lowermost stratospheric ozone losses between 1990 and 2020, with a contribution of inter-halogen ClOx–BrOx cycles to Halog–Loss of approximately 50 %. We conclude that considering the coupling between biogenic bromine sources and seasonal changes of the chlorine heterogeneous reactivation are key features for future projections of mid-latitude lowermost stratospheric ozone during the 21st century.

Javer A. Barrera et al.

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Interactive discussion

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Javer A. Barrera et al.

Javer A. Barrera et al.

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Short summary
The inclusion of biogenic very-short lived bromine (VSLBr) in CAM-Chem model improves the model–satellite agreement of total ozone columns within the mid-latitudes and drives a persistent hemispheric asymmetry in the lowermost stratospheric ozone losses. The seasonal VSLBr impacts show a clear dependence on the heterogeneous reactivation of inorganic chlorine reservoirs occurring in the mid-latitude lowermost stratosphere, with a clear increase in ozone destruction during spring and winter.
The inclusion of biogenic very-short lived bromine (VSLBr) in CAM-Chem model improves the...
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