The 1994 northern midlatitude budget of stratospheric chlorine derived from ATMOS/ATLAS‐3 observations

Abstract

Volume mixing ratio (VMR) profiles of the chlorine‐bearing gases HCl, ClONO2, CCl3F, CCl2F2, CHClF2, CCl4, and CH3Cl have been measured between 3 and 49° northern‐ and 65 to 72° southern latitudes with the Atmospheric Trace MOlecule Spectroscopy (ATMOS) instrument during the ATmospheric Laboratory for Applications and Science (ATLAS)‐3 shuttle mission of 3 to 12 November 1994. A subset of these profiles obtained between 20 and 49°N at sunset, combined with ClO profiles measured by the Millimeter‐wave Atmospheric Sounder (MAS) also from aboard ATLAS‐3, measurements by balloon for HOCl, CH3CCl3 and C2Cl3F3, and model calculations for COClF indicates that the mean burden of chlorine, ClTOT, was equal to (3.53±0.10) ppbv (parts per billion by volume), 1‐sigma, throughout the stratosphere at the time of the ATLAS 3 mission. This is some 37% larger than the mean 2.58 ppbv value measured by ATMOS within the same latitude zone during the Spacelab 3 flight of 29 April to 6 May 1985, consitent with an exponential growth rate of the chlorine loading in the stratosphere equal to 3.3%/yr or a linear increase of 0.10 ppbv/yr over the Spring‐1985 to Fall‐1994 time period. These findings are in agreement with both the burden and increase of the main anthropogenic Cl‐bearing source gases at the surface during the 1980s, confirming that the stratospheric chlorine loading is primarily of anthropogenic origin.