Methyl chloride in the UT/LS observed by CARIBIC: global distribution, Asian summer monsoon outflow, and use as a tracer for tropical air

Tuesday, 16 December 2014
Taku Umezawa1, Angela Kathleen Baker1, David Oram2, Carina Sauvage1, Armin Rauthe-Schoech1, Stephen A Montzka3, Andreas Zahn4 and Carl A M Brenninkmeijer1, (1)Max Planck Institute for Chemistry, Mainz, Germany, (2)University of East Anglia, School of Environmental Sciences, Norwich, United Kingdom, (3)NOAA OAR ESRL GMD, Boulder, CO, United States, (4)Karlsruhe Institute of Technology, Atmospheric trace gas measurements and remote sensing, Karlsruhe, Germany
We present spatiotemporal variations of methyl chloride (CH3Cl) in the UT/LS observed mainly by the CARIBIC passenger aircraft for the years 2005–2011. The CH3Cl mixing ratio in the UT over Europe was higher than that observed at a European surface baseline station year-round, indicative of a persistent positive vertical gradient at NH mid latitudes. A series of flights over Africa and South Asia show that CH3Cl mixing ratios increase toward tropical latitudes, and the observed UT CH3Cl level over these two regions and the Atlantic was higher than that measured at remote surface sites. Strong emissions of CH3Cl in the tropics combined with meridional transport through the UT may explain such vertical and latitudinal gradients. Comparisons with CO data indicate that non-combustion sources in the tropics dominantly contribute to forming the latitudinal gradient of CH3Cl in the UT. We also observed elevated CH3Cl and CO in air influenced by biomass burning in South America and Africa, and the enhancement ratios derived for CH3Cl to CO in those regions agree with previous observations. In contrast, correlations indicate a high CH3Cl to CO ratio of 2.9±0.5 ppt ppb-1 in the Asian summer monsoon anticyclone and domestic biofuel emissions in South Asia are inferred to be responsible. We estimated CH3Cl emissions from South Asia to be 134±23 Gg Cl yr-1, which is higher than a previous estimate due to the higher CH3Cl to CO ratio observed in this study.

We also examine the use of CH3Cl as a tracer of tropical tropospheric air in the LMS, where we identified air masses with elevated CH3Cl that were however stratospheric in terms of N2O. Back trajectories suggest recent low-latitude origins of such air masses in early summer. In this season, high CH3Cl LMS air shows a clear branch connecting stratospheric and tropical tropospheric air on N2O-CH3Cl scatterplots. This distinct feature vanishes in late summer when the LMS is ventilated by tropospheric air.