1Centre for Ocean and Atmospheric Sciences (COAS), School of Environmental Sciences, University of East Anglia, Norwich, NR4 7TJ, UK
2National Center for Atmospheric Science (NCAS), Centre for Ocean and Atmospheric Sciences (COAS), School of Environmental Sciences, University of East Anglia, Norwich, NR4 7TJ, UK
3Royal Netherlands Meteorological Institute (KNMI), P.O. Box 201, 3730 AE, de Bilt, the Netherlands
4Karlsruhe Institute of Technology-Atmospheric Trace Gases and Remote Sensing (IMK-ASF), Postfach 36 40, 76021, Karlsruhe, Germany
5Max Planck Institute for Chemistry, Air Chemistry Division, Hahn-Meitner Weg 1, 55128, Mainz, Germany
Received: 22 Oct 2013 – Discussion started: 15 Nov 2013
Abstract. Short-lived organic brominated compounds make up a significant part of the organic bromine budget in the atmosphere. Emissions of these compounds are highly variable and there are limited measurements, particularly in the extra-tropical upper troposphere/lower stratosphere and tropical troposphere. Measurements of five very short-lived bromomethanes (VSLB) were made in air samples collected on the CARIBIC project aircraft over three flight routes; Germany to Venezuela/Columbia during 2009–2011, Germany to South Africa during 2010 and 2011 and Germany to Thailand/Kuala Lumpur, Malaysia during 2012 and 2013.
Revised: 20 Feb 2014 – Accepted: 21 Feb 2014 – Published: 08 Apr 2014
In the tropical troposphere, as the most important entrance region to the stratosphere, we observe a total mean organic bromine derived from these compounds across all flights at 10–12 km altitude of 3.4 ± 1.5 ppt. Individual mean tropical tropospheric mixing ratios across all flights were 0.43, 0.74, 0.14, 0.23 and 0.11 ppt for CHBr3, CH2Br2, CHBr2Cl, CHBrCl2 and CH2BrCl respectively. The highest levels of VSLB-derived bromine (4.20 ± 0.56 ppt) were observed in flights between Bangkok and Kuala Lumpur indicating that the South China Sea is an important source region for these compounds. Across all routes, CHBr3 and CH2Br2 accounted for 34% (4.7–71) and 48% (14–73) respectively of total bromine derived from the analysed VSLB in the tropical mid-upper troposphere totalling 82% (54–89).
In samples collected between Germany and Venezuela/Columbia, we find decreasing mean mixing ratios with increasing potential temperature in the extra-tropics. Tropical mean mixing ratios are higher than extra-tropical values between 340–350 K indicating that rapid uplift is important in determining mixing ratios in the lower tropical tropopause layer in the West Atlantic tropics.
O3 was used as a tracer for stratospherically influenced air and we detect rapidly decreasing mixing ratios for all VSLB above ∼100 ppb O3 corresponding to the extra-tropical tropopause layer.
Wisher, A., Oram, D. E., Laube, J. C., Mills, G. P., van Velthoven, P., Zahn, A., and Brenninkmeijer, C. A. M.: Very short-lived bromomethanes measured by the CARIBIC observatory over the North Atlantic, Africa and Southeast Asia during 2009–2013, Atmos. Chem. Phys., 14, 3557-3570, doi:10.5194/acp-14-3557-2014, 2014.