Abstract

Abstract. Natural and anthropogenic emissions of primary aerosols and sulphur dioxide (SO2) are estimated for the year 2010 by assimilating daily total and fine mode aerosol optical depth (AOD) at 550 nm from the Moderate Resolution Imaging Spectroradiometer (MODIS) satellite instrument into a global aerosol model of intermediate complexity. The system adjusts monthly emission fluxes over a set of predefined regions tiling the globe. The resulting aerosol emissions improve the model performance, as measured from usual skill scores, both against the assimilated observations and a set of independent ground-based measurements. The estimated emission fluxes are 67 Tg S yr−1 for SO2, 12 Tg yr−1 for black carbon (BC), 87 Tg yr−1 for particulate organic matter (POM), 17 000 Tg yr−1 for sea salt (SS, estimated at 80 % relative humidity) and 1206 Tg yr−1 for desert dust (DD). They represent a difference of +53, +73, +72, +1 and −8%, respectively, with respect to the first guess (FG) values. Constant errors throughout the regions and the year were assigned to the a priori emissions. The analysis errors are reduced with respect to the a priori ones for all species and throughout the year, they vary between 3 and 18% for SO2, 1 and 130% for biomass burning, 21 and 90 % for fossil fuel, 1 and 200% for DD and 1 and 5% for SS. The maximum errors on the global-yearly scale for the estimated fluxes (considering temporal error dependence) are 3% for SO2, 14% for BC, 11% for POM, 14% for DD and 2% for SS. These values represent a decrease as compared to the global-yearly errors from the FG of 7% for SO2, 40% for BC, 55% for POM, 81% for DD and 300% for SS. The largest error reduction, both monthly and yearly, is observed for SS and the smallest one for SO2. The sensitivity and robustness of the inversion system to the choice of the first guess emission inventory is investigated by using different combinations of inventories for industrial, fossil fuel and biomass burning sources. The initial difference in the emissions between the various set-ups is reduced after the inversion. Furthermore, at the global scale, the inversion is sensitive to the choice of the BB (biomass burning) inventory and not so much to the industrial and fossil fuel inventory. At the regional scale, however, the choice of the industrial and fossil fuel inventory can make a difference. The estimated baseline emission fluxes for SO2, BC and POM are within the estimated uncertainties of the four experiments. The resulting emissions were compared against projected emissions for the year 2010 for SO2, BC and POM. The new estimate presents larger emissions than the projections for all three species, with larger differences for SO2 than POM and BC. These projected SO2 emissions are outside the uncertainties of the estimated emission inventories.

Highlights

  • Earth System SciencesAerosols play an important role in air quality, atmospheric visibility and climate

  • In addition to the above-described dataset, we explore the sensitivity of the estimated emissions, on one hand by replacing the GFEDv3 biomass burning emissions with the Global Fire Assimilation System (GFAS) v1.0 inventory (Kaiser et al, 2012), and on the other hand by replacing the Lamarque et al (2010) anthropogenic emissions of SO2, black carbon (BC) and particulate organic matter (POM) with the AeroCom emission inventory of the year 2000 (Diehl et al, 2012)

  • We make use of the tools developed at the Laboratoire des Sciences du Climat et de l’Environnement (LSCE) in the framework of the AeroCom project, which includes a platform for detailed evaluation of aerosol simulation in global models

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Summary

Introduction

Aerosols play an important role in air quality, atmospheric visibility and climate. Concentration levels of particulate mdiactatteorrsbeolfowair2.q5uaalnidtyO1a0ncμdemaaraent kthSneocwsiunerfntaocceheaavree used as inan adverse impact on human health (Keuken et al, 2011; Perez et al., 2010). A significant part of this uncertainty is due to a lack of knowledge on the spatial and temporal distribution of aerosol emissions (Lee et al, 2011) Such knowledge is needed to quantify the impact of aerosols on climate and air quality in regional and global aerosol models. This study builds on the work presented in Huneeus et al (2012), hereafter denoted HCB12, where a detailed description of the assimilation system as well as an assessment of its preliminary application to estimate the aerosol and SO2 emissions for the year 2002 were given. In the present study we have improved our treatment of uncertainties and have updated the a priori emissions inventory and the choice of target regions for the source inversion.

Assimilation system
Assimilation method
Observations
State vector
Error covariances
Emission inventories
Results
Statistical analysis
Emission fluxes
Conclusions
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