ACPD Atmospheric Chemistry and Physics Discussions ACPD 1680-7375 Copernicus GmbH Göttingen, Germany 10.5194/acpd-10-12225-2010 Atmospheric three-dimensional inverse modeling of regional industrial emissions and global oceanic uptake of carbon tetrachloride Xiao X. 1 8 Prinn R. G. 1 Fraser P. J. 2 Weiss R. F. 3 Simmonds P. G. 4 O'Doherty S. 4 Miller B. R. 5 Salameh P. K. 3 Harth C. M. 3 Krummel P. B. 2 Golombek A. 1 Porter L. W. 6 9 Elkins J. W. 5 Dutton G. S. 5 Hall B. D. 5 Steele L. P. 2 Wang R. H. J. 7 Cunnold D. M. 7 9 Department of Earth, Atmospheric, and Planetary Sciences, MIT, Cambridge, MA 02139, USA Centre for Australian Weather and Climate Research, CSIRO Marine and Atmospheric Research, Aspendale, Victoria 3195, Australia Scripps Institution of Oceanography, University of California, San Diego, La Jolla, CA 92093, USA School of Chemistry, University of Bristol, Bristol, UK ESRL, NOAA, Boulder, CO 80305, USA Centre for Australian Weather and Climate Research, Australian Government Bureau of Meteorology, Melbourne, Victoria 3000, Australia School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA 30332, USA now at: Civil & Environmental Engineering, Rice University, Houston, TX 77005, USA deceased 10 05 2010 10 5 12225 12260 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys-discuss.net/10/12225/2010/acpd-10-12225-2010.html The full text article is available as a PDF file from http://www.atmos-chem-phys-discuss.net/10/12225/2010/acpd-10-12225-2010.pdf

Carbon tetrachloride (CCl<sub>4</sub>) has substantial stratospheric ozone depletion potential and its consumption is controlled under the Montreal Protocol and its amendments. We implement a Kalman filter using atmospheric CC1<sub>4</sub> measurements and a 3-dimensional chemical transport model to estimate the interannual regional industrial emissions and seasonal global oceanic uptake of CCl<sub>4</sub> for the period of 1996–2004. The Model of Atmospheric Transport and Chemistry (MATCH), driven by offline National Center for Environmental Prediction (NCEP) reanalysis meteorological fields, is used to simulate CCl<sub>4</sub> mole fractions and calculate their sensitivities to regional sources and sinks using a finite difference approach. High frequency observations from the Advanced Global Atmospheric Gases Experiment (AGAGE) and NOAA Earth System Research Laboratory (ESRL) and low frequency flask observations are together used to constrain the source and sink magnitudes, estimated as factors that multiply the a priori fluxes. Although industry data imply that the global industrial emissions were substantially declining with large interannual variations, the optimized results show only small interannual variations and a small decreasing trend. The global surface CCl<sub>4</sub> mole fractions were declining in this period because the CCl<sub>4</sub> oceanic and stratospheric sinks exceeded the industrial emissions. Compared to the a priori values, the inversion results indicate substantial increases in industrial emissions originating from the South Asian/Indian and Southeast Asian regions, and significant decreases in emissions from the European and North American regions.

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