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trace gas
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Methyl chloride (CH3Cl) is a chlorine-containing trace gas in the atmosphere contributing significantly to stratospheric ozone depletion. Large uncertainties in estimates of its source and sink magnitudes and temporal and spatial variations currently exist. GEIA inventories and other bottom-up emission estimates are used to construct a priori maps of the surface fluxes of CH3Cl. The Model of Atmospheric Transport and Chemistry (MATCH), driven by NCEP interannually varying meteorological data, is then used to simulate CH3Cl mole fractions and quantify the time series of sensitivities of the mole fractions at each measurement site to the surface fluxes of various regional and global sources and sinks. We then implement the Kalman filter (with the unit pulse response method) to estimate the surface fluxes on regional/global scales with monthly resolution from January 2000 to December 2004. High frequency observations from the AGAGE, SOGE, NIES, and NOAA/ESRL HATS in situ networks and low frequency observations from the NOAA/ESRL HATS flask network are used to constrain the source and sink magnitudes. The inversion results indicate global total emissions around 4100 ± 470 Gg yr-1 with very large emissions of 2200 ± 390 Gg yr-1 from tropical plants, which turn out to be the largest single source in the CH3Cl budget. Relative to their a priori annual estimates, the inversion increases global annual fungal and tropical emissions, and reduces the global oceanic source. The inversion implies greater seasonal and interannual oscillations of the natural sources and sink of CH3Cl compared to the a priori. The inversion also reflects the strong effects of the 2002/2003 globally widespread heat waves and droughts on global emissions from tropical plants, biomass burning and salt marshes, and on the soil sink.
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An intensive measurement campaign was performed in June 2000 at the Mt. Cimone station (44°11' N-10°42' E, 2165 m asl, the highest mountain in the northern Italian Apennines) to study photochemical ozone production in the lower free troposphere. In general, average mixing ratios of important trace gases were not very high (121 ± 20 ppbv CO, 0.284 ± 0.220 ppbv NOx, 1.15 ± 0.8 ppbv NOy, 58 ± 9 ppbv O3), which indicates a small contribution by local pollution. Those trace gas levels are representative of continental background air, which is further supported by the analysis of VOCs (e.g.: C2H6 = (905 ± 200) pptv, C3H8 = (268 ±110) pptv, C2H2 = (201 ± 102) pptv, C5H8 = (111 ± 124) pptv, benzene = (65 ± 33) pptv). Furthermore, significant diurnal variations for a number of trace gases (O3, CO, NOx, NOy, HCHO) indicate the presence of free tropospheric airmasses at nighttime as a consequence of local catabatic winds. Average mid-day peroxy radical concentrations at Mt. Cimone are of the order of 30 pptv. At mean NO concentrations of the order of 40 pptv this gives rise to significant in situ net O3 production of 0.1-0.3 ppbv/hr. The importance of O3 production is supported by correlations between O3, CO, NOz, and HCHO, and between HCHO, CO and NOy.