GLOBAL BUDGET OF ATMOSPHERIC ACETONE

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Presentation transcript:

GLOBAL BUDGET OF ATMOSPHERIC ACETONE Singh et al. This work This work [2000] (a priori) (optimized) SOURCES (Tg yr-1) 56 (37-80) 78 (49-105) 95 (80-110) Terrestrial vegetation 15 (10-20) 26 (0-52) 33 (24-42) Plant decay 6 (4-8) 9 (0-18) 2 (-3-7) Biomass burning 5 (3-10) 3 (2-5) 5 (3-7) Industry 2 (1-3) 1 (1-2) 1 (1-2) Oceans 0 10 (0-20) 27 (21-33) Oxidation of isoalkanes 17 (12-24) 20 (10-30) 21 (16-26) Oxidation of terpenes, MBO 11 (7-15) 9 (3-15) 7 (3-11) SINKS (Tg yr-1) 56 (37-80) 78 95 Photolysis 36 (24-51) 44 46 Oxidation by OH 13 (9-19) 25 27 Deposition to land 7 (4-10) 9 9 Uptake by ocean 0 0 14 LIFETIME 16 days 20 days 15 days

ATMOSPHERIC OBSERVATIONS OF ACETONE (0.2-3 ppbv) TRACE-A ABLE -3B Surface sites PEM -WB SONEX PEM-TB

OCEANIC SIGNATURE IN ATMOSPHERIC ACETONE OBSERVATIONS? South Pacific [Singh et al., 2001] southern Sweden [Solberg et al., 1996] Low winter values over Europe: ocean sink? High values over South Pacific: ocean source?

ROLE OF OCEAN IN ATMOSPHERIC BUDGET OF ACETONE Biological uptake (Kieber et al., 1990) SINK? H298 = 30 M atm-1; physical uptake limited by both gas- and aqueous-phase transfer hn SOURCE? Zhou and Mopper (1997) Organic microlayer organic microlayer Model sink as adjustable saturation ratio R Model source as proportional To UV-B flux

INVERSE MODEL ANALYSIS OF ACETONE BUDGET Global 3-D model (“forward model”): defines sensitivity of atmospheric concentrations to global sources/sinks (“state vector”) A priori best estimate of sources/sinks (with errors) Observed atmospheric concentrations (with “errors”) A posteriori optimized estimate of sources/sinks

CONSTRUCTING THE A PRIORI: SIMULATION OF C3-5 ISOALKANES TO IMPROVE CONSTRAINT ON EMISSIONS observed model (EDGAR) model (Piccot+) Global propane source of 12 Tg C yr-1, mainly natural gas

CONTRIBUTION OF DIFFERENT SOURCES TO A PRIORI BUDGET OF ACETONE (symbols: observations lines: model)

FITTING OF OCEAN SATURATION RATIO R TO MINIMIZE MODEL vs FITTING OF OCEAN SATURATION RATIO R TO MINIMIZE MODEL vs. OBSERVED CHI-SQUARE IN A POSTERIORI OPTIMIZED SOURCES Best fit for R = 0.7-0.85

OPTIMIZED GLOBAL 3-D MODEL SIMULATION OF ATMOSPHERIC ACETONE a priori sources/sinks; c2 = 1.3 Optimized sources/sinks (including “microbial” ocean sink, photochemical ocean source); c2 = 0.39

SURFACE AIR ACETONE CONCENTRATIONS IN OPTIMIZED SIMULATION