Abstract
The atmospheric budget and distribution of acetone are investigated by using a priori estimates of sources and sinks to constrain a global three‐dimensional atmospheric model simulation and then using atmospheric observations from 14 surface sites and 5 aircraft missions to improve these estimates through an inversion analysis. Observations over the South Pacific imply a large photochemical marine source of acetone, either from the ocean or from marine organic aerosol. Low concentrations of acetone measured at European sites in winter‐spring and in the Arctic in summer suggest a large microbial ocean sink. The summer‐to‐fall decrease of concentrations observed in Europe argues against a large source from plant decay. Continental observations in the tropics and at northern midlatitudes in summer imply a large source from terrestrial vegetation. Observations in the Northern Hemisphere outside summer imply a large source from atmospheric oxidation of anthropogenic isoalkanes (propane, isobutane, isopentane). Model simulation of isoalkanes and comparison to observations yields best global emission estimates of 12 Tg C yr−1 for propane (including only 0.6 Tg C yr−1 from biomass burning), 3.6 Tg C yr−1 for isobutane, and 5.0 Tg C yr−1 for isopentane. Our best estimate of the global acetone source is 95 Tg yr−1. The mean tropospheric lifetime of acetone is estimated to be 15 days. Terrestrial vegetation and oceans are the principal sources of acetone in the tropopause region (0.1–0.7 ppbv) except in the extratropical Northern Hemisphere, where oxidation of isoalkanes is more important.
Highlights
[1] The atmospheric budget and distribution of acetone are investigated by using a priori estimates of sources and sinks to constrain a global three-dimensional atmospheric model simulation and using atmospheric observations from 14 surface sites and 5 aircraft missions to improve these estimates through an inversion analysis
Photolysis of acetone in the upper troposphere is a major source of hydrogen oxide radicals (HOx = OH + peroxy radicals) and peroxyacetylnitrate (PAN), with important implications for global tropospheric chemistry [Singh et al, 1995; Jaegleet al., 1997, 2001; McKeen et al, 1997; Wennberg et al, 1998; Collins et al, 1999; Muller and Brasseur, 1999]
In the present paper we use a global three-dimensional (3-D) model simulation to examine the consistency between these atmospheric measurements and our current understanding of acetone sources
Summary
[2] Acetone is present ubiquitously in the troposphere at concentrations in the range 0.2 – 3 ppbv [Singh et al, 1994, 1995, 2000, 2001; Arnold et al, 1997; Wohlfrom et al, 1999]. Sinks include photolysis and reaction with OH, resulting in a global mean lifetime for acetone of the order of a month [Gierczak et al, 1998]. Atmospheric measurements of acetone concentrations have been made at a number of surface sites and during aircraft campaigns over the past decade (Table 2). In the present paper we use a global three-dimensional (3-D) model simulation to examine the consistency between these atmospheric measurements and our current understanding of acetone sources
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