Abstract. We use 2010–2015 observations of atmospheric methane columns from the GOSAT satellite instrument in a global inverse analysis to improve estimates of methane emissions and their trends over the period, as well as the global concentration of tropospheric OH (the hydroxyl radical, methane's main sink) and its trend. Our inversion solves the Bayesian optimization problem analytically including closed-form characterization of errors. This allows us to (1) quantify the information content from the inversion towards optimizing methane emissions and its trends, (2) diagnose error correlations between constraints on emissions and OH concentrations, and (3) generate a large ensemble of solutions testing different assumptions in the inversion. We show how the analytical approach can be used, even when prior error standard deviation distributions are lognormal. Inversion results show large overestimates of Chinese coal emissions and Middle East oil and gas emissions in the EDGAR v4.3.2 inventory but little error in the United States where we use a new gridded version of the EPA national greenhouse gas inventory as prior estimate. Oil and gas emissions in the EDGAR v4.3.2 inventory show large differences with national totals reported to the United Nations Framework Convention on Climate Change (UNFCCC), and our inversion is generally more consistent with the UNFCCC data. The observed 2010–2015 growth in atmospheric methane is attributed mostly to an increase in emissions from India, China, and areas with large tropical wetlands. The contribution from OH trends is small in comparison. We find that the inversion provides strong independent constraints on global methane emissions (546 Tg a−1) and global mean OH concentrations (atmospheric methane lifetime against oxidation by tropospheric OH of 10.8±0.4 years), indicating that satellite observations of atmospheric methane could provide a proxy for OH concentrations in the future.

Emissions from 15 agricultural fires in the southeastern U.S. were measured from the NASA DC‐8 research aircraft during the summer 2013 Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) campaign. This study reports a detailed set of emission factors (EFs) for 25 trace gases and 6 fine particle species. The chemical evolution of the primary emissions in seven plumes was examined in detail for ~1.2 h. A Lagrangian plume cross‐section model was used to simulate the evolution of ozone (O3), reactive nitrogen species, and organic aerosol (OA). Observed EFs are generally consistent with previous measurements of crop residue burning, but the fires studied here emitted high amounts of SO2 and fine particles, especially primary OA and chloride. Filter‐based measurements of aerosol light absorption implied that brown carbon (BrC) was ubiquitous in the plumes. In aged plumes, rapid production of O3, peroxyacetyl nitrate (PAN), and nitrate was observed with ΔO3/ΔCO, ΔPAN/ΔNOy, and Δnitrate/ΔNOy reaching ~0.1, ~0.3, and ~0.3. For five selected cases, the model reasonably simulated O3 formation but underestimated PAN formation. No significant evolution of OA mass or BrC absorption was observed. However, a consistent increase in oxygen‐to‐carbon (O/C) ratios of OA indicated that OA oxidation in the agricultural fire plumes was much faster than in urban and forest fire plumes. Finally, total annual SO2, NOx, and CO emissions from agricultural fires in Arkansas, Louisiana, Mississippi, and Missouri were estimated (within a factor of ~2) to be equivalent to ~2% SO2 from coal combustion and ~1% NOx and ~9% CO from mobile sources.

Abstract. Fine particulate matter (PM2.5) is a severe air pollution problem in China. Observations of PM2.5 have been available since 2013 from a large network operated by the China National Environmental Monitoring Center (CNEMC). The data show a general 30 %–50 % decrease in annual mean PM2.5 across China over the 2013–2018 period, averaging at −5.2 µg m−3 a−1. Trends in the five megacity cluster regions targeted by the government for air quality control are -9.3±1.8 µg m−3 a−1 (±95 % confidence interval) for Beijing–Tianjin–Hebei, -6.1±1.1 µg m−3 a−1 for the Yangtze River Delta, -2.7±0.8 µg m−3 a−1 for the Pearl River Delta, -6.7±1.3 µg m−3 a−1 for the Sichuan Basin, and -6.5±2.5 µg m−3 a−1 for the Fenwei Plain (Xi'an). Concurrent 2013–2018 observations of sulfur dioxide (SO2) and carbon monoxide (CO) show that the declines in PM2.5 are qualitatively consistent with drastic controls of emissions from coal combustion. However, there is also a large meteorologically driven interannual variability in PM2.5 that complicates trend attribution. We used a stepwise multiple linear regression (MLR) model to quantify this meteorological contribution to the PM2.5 trends across China. The MLR model correlates the 10 d PM2.5 anomalies to wind speed, precipitation, relative humidity, temperature, and 850 hPa meridional wind velocity (V850). The meteorology-corrected PM2.5 trends after removal of the MLR meteorological contribution can be viewed as being driven by trends in anthropogenic emissions. The mean PM2.5 decrease across China is −4.6 µg m−3 a−1 in the meteorology-corrected data, 12 % weaker than in the original data, meaning that 12 % of the PM2.5 decrease in the original data is attributable to meteorology. The trends in the meteorology-corrected data for the five megacity clusters are -8.0±1.1 µg m−3 a−1 for Beijing–Tianjin–Hebei (14 % weaker than in the original data), -6.3±0.9 µg m−3 a−1 for the Yangtze River Delta (3 % stronger), -2.2±0.5 µg m−3 a−1 for the Pearl River Delta (19 % weaker), -4.9±0.9 µg m−3 a−1 for the Sichuan Basin (27 % weaker), and -5.0±1.9 µg m−3 a−1 for the Fenwei Plain (Xi'an; 23 % weaker); 2015–2017 observations of flattening PM2.5 in the Pearl River Delta and increases in the Fenwei Plain can be attributed to meteorology rather than to relaxation of emission controls.

Cryospheric forcing, that is, decreasing Arctic sea ice and increasing Eurasia snow, exacerbated extreme winter haze in China.

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Abstract. The chemical mechanisms responsible for rapid sulfate production, an important driver of winter haze formation in northern China, remain unclear. Here, we propose a potentially important heterogeneous hydroxymethanesulfonate (HMS) chemical mechanism. Through analyzing field measurements with aerosol mass spectrometry, we show evidence for a possible significant existence in haze aerosols of organosulfur primarily as HMS, misidentified as sulfate in previous observations. We estimate that HMS can account for up to about one-third of the sulfate concentrations unexplained by current air quality models. Heterogeneous production of HMS by SO2 and formaldehyde is favored under northern China winter haze conditions due to high aerosol water content, moderately acidic pH values, high gaseous precursor levels, and low temperature. These analyses identify an unappreciated importance of formaldehyde in secondary aerosol formation and call for more research on sources and on the chemistry of formaldehyde in northern China winter.

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Abstract. We conduct a global inverse analysis of 2010–2018 GOSAT observations to better understand the factors controlling atmospheric methane and its accelerating increase over the 2010–2018 period. The inversion optimizes anthropogenic methane emissions and their 2010–2018 trends on a 4∘×5∘ grid, monthly regional wetland emissions, and annual hemispheric concentrations of tropospheric OH (the main sink of methane). We use an analytical solution to the Bayesian optimization problem that provides closed-form estimates of error covariances and information content for the solution. We verify our inversion results with independent methane observations from the TCCON and NOAA networks. Our inversion successfully reproduces the interannual variability of the methane growth rate inferred from NOAA background sites. We find that prior estimates of fuel-related emissions reported by individual countries to the United Nations are too high for China (coal) and Russia (oil and gas) and too low for Venezuela (oil and gas) and the US (oil and gas). We show large 2010–2018 increases in anthropogenic methane emissions over South Asia, tropical Africa, and Brazil, coincident with rapidly growing livestock populations in these regions. We do not find a significant trend in anthropogenic emissions over regions with high rates of production or use of fossil methane, including the US, Russia, and Europe. Our results indicate that the peak methane growth rates in 2014–2015 are driven by low OH concentrations (2014) and high fire emissions (2015), while strong emissions from tropical (Amazon and tropical Africa) and boreal (Eurasia) wetlands combined with increasing anthropogenic emissions drive high growth rates in 2016–2018. Our best estimate is that OH did not contribute significantly to the 2010–2018 methane trend other than the 2014 spike, though error correlation with global anthropogenic emissions limits confidence in this result.