Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 9 12 2009 10.5194/acp-9-3911-2009 http://www.atmos-chem-phys.net/9/3911/2009/ http://www.atmos-chem-phys.net/9/3911/2009/acp-9-3911-2009.html http://www.atmos-chem-phys.net/9/3911/2009/acp-9-3911-2009.pdf 3911 3934 2009-06-17 Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn P. Martinerie patricia@lgge.obs.ujf-grenoble.fr E. Nourtier-Mazauric J.-M. Barnola W. T. Sturges D. R. Worton E. Atlas L. K. Gohar K. P. Shine G. P. Brasseur Laboratoire de Glaciologie et Géophysique de l'Environnement (UMR CNRS/INSU 5183), CNRS, Université Joseph Fourier-Grenoble, BP 96, 38 402 Saint Martin d'Hères, France School of Environmental Sciences, University of East Anglia, Norwich, NR4 7TJ, UK Rosenstiel School of Marine and Atmospheric Science, University of Miami, Miami, FL 33149, USA Department of Meteorology, University of Reading, Reading RG6 6BB, UK National Center for Atmospheric Research, Boulder, CO 80307-3000, USA now at: Department of Environmental Science, Policy and Management, University of California, Berkeley, CA 94720-3110, USA now at: Met Office Hadley Centre, FitzRoy Road, Exeter. EX1 3PB, UK The budgets of seven halogenated gases (CFC-11, CFC-12, CFC-113, CFC-114, CFC-115, CCl₄ and SF₆) are studied by comparing measurements in polar firn air from two Arctic and three Antarctic sites, and simulation results of two numerical models: a 2-D atmospheric chemistry model and a 1-D firn diffusion model. The first one is used to calculate atmospheric concentrations from emission trends based on industrial inventories; the calculated concentration trends are used by the second one to produce depth concentration profiles in the firn. The 2-D atmospheric model is validated in the boundary layer by comparison with atmospheric station measurements, and vertically for CFC-12 by comparison with balloon and FTIR measurements. Firn air measurements provide constraints on historical atmospheric concentrations over the last century. Age distributions in the firn are discussed using a Green function approach. Finally, our results are used as input to a radiative model in order to evaluate the radiative forcing of our target gases. Multi-species and multi-site firn air studies allow to better constrain atmospheric trends. The low concentrations of all studied gases at the bottom of the firn, and their consistency with our model results confirm that their natural sources are small. 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