Abstract

Abstract. Comparison between the CMAQ (Community Multi-scale Air Quality Model)-calculated and OMI (Ozone Monitoring Instrument)-retrieved tropospheric NO2 columns was carried out for 2006 over East Asia (100–150° E; 20–50° N) to evaluate the bottom-up NOx emission fluxes of INTEX-B, CAPSS, and REAS v1.11 inventories. The three emission inventories were applied to the CMAQ model simulations for the countries of China, South Korea, and Japan, respectively. For the direct comparison between the two NO2 columns, the averaging kernels (AKs) obtained from the Royal Netherlands Meteorological Institute (KNMI)/DOMINO v2.0 daily product were applied to the CMAQ-simulated data. The analysis showed that the two tropospheric NO2 columns from the CMAQ model simulations and OMI observations (ΩCMAQ,AK and ΩOMI) had good spatial and seasonal correlation, with correlation coefficients ranging from 0.71 to 0.96. In addition, the normalized mean errors (NMEs) between the ΩCMAQ,AK and ΩOMI were found to range from ~ 40 to ~ 63%. The ΩCMAQ,AK were, on annual average, ~ 28% smaller (in terms of the NMEs) than the ΩOMI, indicating that the NOx emissions used were possibly underestimated in East Asia. Large absolute differences between the ΩCMAQ,AK and ΩOMI were found, particularly over central eastern China (CEC) during winter (annual averaged mean error of ~ 4.51 × 1015 molecules cm−2). Although such differences between the ΩCMAQ,AK and ΩOMI are likely caused by the errors and biases in the NOx emissions used in the CMAQ model simulations, it can be rather difficult to quantitatively relate the differences to the accuracy of the NOx emissions, because there are also several uncertain factors in the CMAQ model, satellite-retrieved NO2 columns and AK products, and NOx and other trace gas emissions. In this context, three uncertain factors were selected and analyzed with sensitivity runs (monthly variations in NOx emissions; influences of different NOx emission fluxes; and reaction probability of N2O5 radicals). Other uncertain or possible influential factors were also discussed to suggest future direction of the study.

Highlights

  • There has been growing public concern about serious smog events in East Asia due to large amounts of anthropogenic pollutants in the atmosphere

  • The accuracy of bottom-up NOx emission fluxes from the INTEX-B, CAPSS, and REAS emission inventories were investigated through comparisons between the CMAQ,averaging kernels (AKs) and Ozone Monitoring Instrument (OMI) in East Asia

  • For the direct comparison between the CMAQ and OMI, we applied the AKs to the CMAQ model simulations

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Summary

Introduction

There has been growing public concern about serious smog events in East Asia due to large amounts of anthropogenic pollutants in the atmosphere. Nitrogen oxides (NOx ∼= NO + NO2) play a key role in tropospheric chemistry, such as ozone and secondary aerosol formation. In global climate change, atmospheric NOx is believed to make indirect negative contributions to radiative forcing in the atmosphere (Wild et al, 2001). Secondary nitrates (NO−3 ) formed via the condensation of atmospheric HNO3, NO3, and N2O5 into particles contribute, on average, 30.7 % to aerosol direct radiative forcing (ADRF) in East. Han et al.: Tropospheric NO2 columns over East Asia

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