TY - JOUR

T1 - Recent Trends in Stratospheric Chlorine from Very Short-Lived Substances

AU - Hossaini, Ryan

AU - Atlas, Elliot

AU - Dhomse, Sandip S.

AU - Chipperfield, Martyn P.

AU - Bernath, Peter F.

AU - Fernando, Anton M.

AU - Mühle, Jens

AU - Leeson, Amber A.

AU - Montzka, Stephen A.

AU - Feng, Wuhu

AU - Harrison, Jeremy J.

AU - Krummel, Paul

AU - Vollmer, Martin K.

AU - Reimann, Stefan

AU - O'Doherty, Simon

AU - Young, Dickon

AU - Maione, Michela

AU - Arduini, Jgor

AU - Lunder, Chris R.

PY - 2019/2/27

Y1 - 2019/2/27

N2 - 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.

AB - 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.

KW - chlorine

KW - stratosphere

KW - vsls

KW - chloroform

KW - dichloromethane

KW - ozone

U2 - 10.1029/2018JD029400

DO - 10.1029/2018JD029400

M3 - Journal article

VL - 124

SP - 2318

EP - 2335

JO - Journal of Geophysical Research: Atmospheres

JF - Journal of Geophysical Research: Atmospheres

SN - 0747-7309

IS - 4

ER -