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Abstract. We apply airborne measurements across three seasons(summer, winter and spring 2017–2018) in a multi-inversion framework toquantify methane emissions from the US Corn Belt and Upper Midwest, a keyagricultural and wetland source region. Combing our seasonal results withprior fall values we find that wetlands are the largest regional methanesource (32 %, 20 [16–23] Gg/d), while livestock (enteric/manure; 25 %,15 [14–17] Gg/d) are the largest anthropogenic source. Naturalgas/petroleum, waste/landfills, and coal mines collectively make up theremainder. Optimized fluxes improve model agreement with independentdatasets within and beyond the study timeframe. Inversions reveal coherentand seasonally dependent spatial errors in the WetCHARTs ensemble meanwetland emissions, with an underestimate for the Prairie Pothole region butan overestimate for Great Lakes coastal wetlands. Wetland extent andemission temperature dependence have the largest influence on predictionaccuracy; better representation of coupled soil temperature–hydrologyeffects is therefore needed. Our optimized regional livestock emissionsagree well with the Gridded EPA estimates during spring (to within 7 %) butare ∼ 25 % higher during summer and winter. Spatial analysisfurther shows good top-down and bottom-up agreement for beef facilities (withmainly enteric emissions) but larger (∼ 30 %) seasonaldiscrepancies for dairies and hog farms (with > 40 % manureemissions). Findings thus support bottom-up enteric emission estimates butsuggest errors for manure; we propose that the latter reflects inadequatetreatment of management factors including field application. Overall, ourresults confirm the importance of intensive animal agriculture for regionalmethane emissions, implying substantial mitigation opportunities throughimproved management. 

Abstract. Organic aerosol (OA), with a large biogenic fraction in the summertime southeast US, adversely impacts air quality and human health. Stringent airquality controls have recently reduced anthropogenic pollutants including sulfate, whose impact on OA remains unclear. Three filter measurementnetworks provide long-term constraints on the sensitivity of OA to changes in inorganic species, including sulfate and ammonia. The 2000–2013summertime OA decreases by 1.7 % yr−1–1.9 % yr−1 with little month-to-month variability, while sulfatedeclines rapidly with significant monthly difference in the early 2000s. In contrast, modeled OA from a chemical-transport model (GEOS-Chem) decreasesby 4.9 % yr−1 with much larger monthly variability, largely due to the predominant role of acid-catalyzed reactive uptake ofepoxydiols (IEPOX) onto sulfate. The overestimated modeled OA dependence on sulfate can be improved by implementing a coating effect and assumingconstant aerosol acidity, suggesting the needs to revisit IEPOX reactive uptake in current models. Our work highlights the importance of secondaryOA formation pathways that are weakly dependent on inorganic aerosol in a region that is heavily influenced by both biogenic and anthropogenicemissions. 

ABSTRACT To explore the various couplings across space and time and between ecosystems in a consistent manner, atmospheric modeling is moving away from the fractured limited-scale modeling strategy of the past toward a unification of the range of scales inherent in the Earth system. This paper describes the forward-looking Multi-Scale Infrastructure for Chemistry and Aerosols (MUSICA), which is intended to become the next-generation community infrastructure for research involving atmospheric chemistry and aerosols. MUSICA will be developed collaboratively by the National Center for Atmospheric Research (NCAR) and university and government researchers, with the goal of serving the international research and applications communities. The capability of unifying various spatiotemporal scales, coupling to other Earth system components, and process-level modularization will allow advances in both fundamental and applied research in atmospheric composition, air quality, and climate and is also envisioned to become a platform that addresses the needs of policy makers and stakeholders. 

Abstract. Anthropogenic secondary organic aerosol (ASOA), formed from anthropogenicemissions of organic compounds, constitutes a substantial fraction of themass of submicron aerosol in populated areas around the world andcontributes to poor air quality and premature mortality. However, theprecursor sources of ASOA are poorly understood, and there are largeuncertainties in the health benefits that might accrue from reducinganthropogenic organic emissions. We show that the production of ASOA in 11urban areas on three continents is strongly correlated with the reactivityof specific anthropogenic volatile organic compounds. The differences inASOA production across different cities can be explained by differences inthe emissions of aromatics and intermediate- and semi-volatile organiccompounds, indicating the importance of controlling these ASOA precursors.With an improved model representation of ASOA driven by the observations,we attribute 340 000 PM2.5-related premature deaths per year to ASOA, which isover an order of magnitude higher than prior studies. A sensitivity casewith a more recently proposed model for attributing mortality to PM2.5(the Global Exposure Mortality Model) results in up to 900 000 deaths. Alimitation of this study is the extrapolation from cities with detailedstudies and regions where detailed emission inventories are available toother regions where uncertainties in emissions are larger. In addition tofurther development of institutional air quality management infrastructure,comprehensive air quality campaigns in the countries in South and CentralAmerica, Africa, South Asia, and the Middle East are needed for furtherprogress in this area.