Recent Trends in Stratospheric Chlorine from Very Short-Lived Substances

Hossaini, Ryan and Atlas, Elliot and Dhomse, Sandip S. and Chipperfield, Martyn P. and Bernath, Peter F. and Fernando, Anton M. and Mühle, Jens and Leeson, Amber A. and Montzka, Stephen A. and Feng, Wuhu and Harrison, Jeremy J. and Krummel, Paul and Vollmer, Martin K. and Reimann, Stefan and O'Doherty, Simon and Young, Dickon and Maione, Michela and Arduini, Jgor and Lunder, Chris R. (2019) Recent Trends in Stratospheric Chlorine from Very Short-Lived Substances. Journal of Geophysical Research: Atmospheres, 124 (4). pp. 2318-2335. ISSN 0747-7309

Abstract

Abstract Very short-lived substances (VSLS), including dichloromethane (CH2Cl2), chloroform (CHCl3), perchloroethylene (C2Cl4) and 1,2-dichloroethane (C2H4Cl2), are a stratospheric chlorine source and therefore contribute to ozone depletion. We quantify stratospheric chlorine trends from these VSLS (VSLCltot) using a chemical transport model and atmospheric measurements, including novel high-altitude aircraft data from the NASA VIRGAS (2015) and POSIDON (2016) missions. We estimate VSLCltot increased from 69 (±14) ppt Cl in 2000 to 111 (±22) ppt Cl in 2017, with >80% delivered to the stratosphere through source gas injection (SGI), and the remainder from product gases. The modelled evolution of chlorine SGI agrees well with historical aircraft data, which corroborate reported surface CH2Cl2 increases since the mid-2000s. The relative contribution of VSLS to total stratospheric chlorine increased from ~2% in 2000 to ~3.4% in 2017, reflecting both VSLS growth and decreases in long-lived halocarbons. We derive a mean VSLCltot growth rate of 3.8 (±0.3) ppt Cl/yr between 2004-2017, though year-to-year growth rates are variable and were small or negative in the period 2015-2017. Whether this is a transient effect, or longer-term stabilization, requires monitoring. In the upper stratosphere, the modelled rate of HCl decline (2004-2017) is -5.2 decade with VSLS included, in good agreement to ACE satellite data (-4.8 decade), and 15% slower than a model simulation without VSLS. Thus, VSLS have offset a portion of stratospheric chlorine reductions since the mid-2000s.