Assimilation of POLDER observations to estimate aerosol emissions

Abstract

We apply a local ensemble transform Kalman smoother (LETKS) in combination with the global aerosol-climate model ECHAM-HAM to estimate aerosol emissions from POLDER-3/PARASOL (POLarization and Directionality of the Earth's Reflectances) observations for the year 2006. We assimilate aerosol optical depth at 550gmnm (AOD550), the Ångström exponent at 550 and 865gnm (AE550-865), and single-scattering albedo at 550gnm (SSA550) in order to improve modeled aerosol mass, size and absorption simultaneously. The new global aerosol emissions increase to 1419gTgyr-1 (+28g%) for dust, 1850gTgyr-1 (+75g%) for sea salt, 215gTgyr-1 (+143g%) for organic aerosol and 13.3gTgyr-1 (+75g%) for black carbon, while the sulfur dioxide emissions increase to 198gTgyr-1 (+42g%) and the total deposition of sulfates to 293gTgyr-1 (+39g%). Organic and black carbon emissions are much higher than their prior values from bottom-up inventories, with a stronger increase in biomass burning sources (+193g% and +90g%) than in anthropogenic sources (115g% and 70g%). The evaluation of the experiments with POLDER (assimilated) and AERONET as well as MODIS Dark Target (independent) observations shows a clear improvement compared with the ECHAM-HAM control run. Specifically based on AERONET, the global mean error in AOD550 improves from-0.094 to-0.006, while absorption aerosol optical depth at 550gnm (AAOD550) improves from-0.009 to-0.004 after the assimilation. A smaller improvement is also observed in the AE550-865 mean absolute error (from 0.428 to 0.393), with a considerably higher improvement over isolated island sites at the ocean. The new dust emissions are closer to the ensemble median of AEROCOM I, AEROCOM III and CMIP5 as well as some of the previous assimilation studies. The new sea salt emissions have become closer to the reported emissions from previous studies. Indications of a missing fraction of coarse dust and sea salt particles are discussed. The biomass burning changes (based on POLDER) can be used as alternative biomass burning scaling factors for the Global Fire Assimilation System (GFAS) inventory distinctively estimated for organic carbon (2.93) and black carbon (1.90) instead of the recommended scaling of 3.4 (Kaiser et al., 2012). The estimated emissions are highly sensitive to the relative humidity due to aerosol water uptake, especially in the case of sulfates. We found that ECHAM-HAM, like most of the global climate models (GCMs) that participated in AEROCOM and CMIP6, overestimated the relative humidity compared with ERA5 and as a result the water uptake by aerosols, assuming the kappa values are not underestimated. If we use the ERA5 relative humidity, sulfate emissions must be further increased, as modeled sulfate AOD is lowered. Specifically, over East Asia, the lower AOD can be attributed to the underestimated precipitation and the lack of simulated nitrates in the model.