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Top-down observational constraints on emissions flux estimates from satellite observations of chemical composition are subject to biases and errors stemming from transport, chemistry and prior emissions estimates. In this context, we developed an ensemble data assimilation system to optimize the initial conditions for carbon monoxide (CO) and aerosols, while also quantifying the respective emission fluxes with a distinct attribution of anthropogenic and wildfire sources. We present the separate assimilation of CO profile v9 retrievals from the Measurements of Pollution in the Troposphere (MOPITT) instrument and Aerosol Optical Depth (AOD), collection 6.1, from the Moderate Resolution Imaging Spectroradiometer (MODIS) instruments. This assimilation system is built on the Data Assimilation Research Testbed (DART) and includes a meteorological ensemble to assimilate weather observations within the online Community Atmosphere Model with Chemistry (CAM-chem). Inversions indicate an underestimation of CO emissions in CAMS-GLOB-ANT_v5.1 in China for 2015 and an overestimation of CO emissions in the Fire INventory from NCAR (FINN) version 2.2, especially in the tropics. These emissions increments are consistent between the MODIS AOD and the MOPITT CO-based inversions. Additional simulations and comparison with in situ observations from the NASA Atmospheric Tomography Mission (ATom) show that biases in hydroxyl radical (OH) chemistry dominate the CO errors.

Abstract An ensemble Kalman filter reanalysis has been archived in the Research Data Archive at the National Center for Atmospheric Research. It used a CAM6 configuration of the Community Earth System Model (CESM), several million observations per day, and the Data Assimilation Research Testbed (DART). The data saved from this global, $$\sim 1^\circ $$ ∼ 1 ∘ resolution, 80 member ensemble span 2011–2019. They include ensembles of: sub-daily, real world, atmospheric forcing for use by all of the nonatmospheric models of CESM; weekly, CAM6, restart file sets; 6 hourly, prior hindcast estimates of the assimilated observations; 6 hourly, land model, plant growth variables, and 6 hourly, ensemble mean, gridded, atmospheric analyses. This data can be used for hindcast studies and data assimilation using component models of CESM; CAM6, CLM5, CICE5, POP2. MOM6, MOSART, and CISM; and non-CESM Earth system models. This large dataset (~ 120 Tb) has a unique combination of a large ensemble, high frequency, and multiyear time span, which provides opportunities for robust statistical analysis and use as a machine learning training dataset.