Improved inverse modeling of nitrogen oxides emissions using satellite measurements over China and evidence of volatile organics emissions over the tropical Pacific
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We improved the assimilated daily inversion method by conducting model simulation, satellite retrieval, and inverse modeling sequentially on a daily basis. The improved procedure was applied to GOME-2 and OMI NO₂ measurements over China in 2011, respectively. The new daily retrieval-inversion method significantly reduced the systematic bias in inverse modeling of NOₓ emission between using GOME-2 and OMI measurements, and detected more clear seasonal and weekly variations. OMI instrument observed NO₂ columns over China from 2005 to 2010 were analyzed in order to estimate the top-down anthropogenic NOₓ emission trends. The estimated average emission trend is slower than the trend reported for previous years. We find large regional, seasonal, and urban-rural variations in emission trends. These results appear to suggest that a number of factors have significantly reduced or even reversed the increasing trend of NOₓ emissions in more economically developed megacities and southern coastal regions, but their effects are not as significant in other major cities or less economically developed regions. A 1-D chemical transport model was applied to analyze OH and HO₂ radical observations during the Pacific Atmospheric Sulfur Experiment (PASE) near Christmas Island (Kiritimati, 1.52°N 157.24°W) from Aug. 2 through Sep. 10, 2007. In two of fourteen research flights, significantly higher HO₂/OH ratios in the buffer layer than the other flights were found. Model simulations indicated that fast-reacting oxygenated volatile organic compounds, which can react rapidly with OH and provide additional primary radical sources through photolysis, were necessary to explain the observations. During or right before these two flights, the WRF model simulated two strongest shallow convective events during this experiment, suggesting a transport pathway of ocean organics into the buffer layer. Ocean upwelling driven by atmospheric pressure depression during convection may expedite the release of ocean organics.