Abstract

Abstract. We conducted long-term network observations using standardized Multi-Axis Differential optical absorption spectroscopy (MAX-DOAS) instruments in Russia and ASia (MADRAS) from 2007 onwards and made the first synthetic data analysis. At seven locations (Cape Hedo, Fukue and Yokosuka in Japan, Hefei in China, Gwangju in Korea, and Tomsk and Zvenigorod in Russia) with different levels of pollution, we obtained 80 927 retrievals of tropospheric NO2 vertical column density (TropoNO2VCD) and aerosol optical depth (AOD). In the technique, the optimal estimation of the TropoNO2VCD and its profile was performed using aerosol information derived from O4 absorbances simultaneously observed at 460–490 nm. This large data set was used to analyze NO2 climatology systematically, including temporal variations from the seasonal to the diurnal scale. The results were compared with Ozone Monitoring Instrument (OMI) satellite observations and global model simulations. Two NO2 retrievals of OMI satellite data (NASA ver. 2.1 and Dutch OMI NO2 (DOMINO) ver. 2.0) generally showed close correlations with those derived from MAX-DOAS observations, but had low biases of up to ~50%. The bias was distinct when NO2 was abundantly present near the surface and when the AOD was high, suggesting a possibility of incomplete accounting of NO2 near the surface under relatively high aerosol conditions for the satellite observations. Except for constant biases, the satellite observations showed nearly perfect seasonal agreement with MAX-DOAS observations, suggesting that the analysis of seasonal features of the satellite data were robust. Weekend reduction in the TropoNO2VCD found at Yokosuka and Gwangju was absent at Hefei, implying that the major sources had different weekly variation patterns. While the TropoNO2VCD generally decreased during the midday hours, it increased exceptionally at urban/suburban locations (Yokosuka, Gwangju, and Hefei) during winter. A global chemical transport model, MIROC-ESM-CHEM (Model for Interdisciplinary Research on Climate–Earth System Model–Chemistry), was validated for the first time with respect to background NO2 column densities during summer at Cape Hedo and Fukue in the clean marine atmosphere.

Highlights

  • Nitrogen oxides (NOx), i.e., NO and NO2, are key chemical species in driving tropospheric photochemistry, and they participate in the mechanisms used to explain local–global air pollution

  • We focus on NO2 in this paper, so the evaluation of our aerosol optical depth (AOD) results is included in the Supplement

  • The NO2 data obtained at Yokosuka and Hedo have been partly used for validation of TropoNO2VCD derived from Ozone Monitoring Instrument (OMI) and other satellite sensors (Irie et al, 2009, 2012), comparisons with ship-based observations (Takashima et al, 2012), and for analysis of transport from the Asian continent (Takashima et al, 2011)

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Summary

Introduction

Nitrogen oxides (NOx), i.e., NO and NO2, are key chemical species in driving tropospheric photochemistry, and they participate in the mechanisms used to explain local–global air pollution. They are originally emitted or produced from natural (soil and lightning) and anthropogenic sources, and are strongly involved in the chain reactions forming tropospheric ozone (O3). The reaction of NO with peroxy radicals (HO2 and organic peroxy radicals, RO2) produces NO2, resulting in net production of O3 via subsequent photolysis of NO2 This reaction simultaneously recycles OH radicals, which determine the atmospheric oxidative capacity, and this sustains the concentration levels of peroxy radicals. Knowledge of global and regional distributions of NO2, their temporal variations, and the underlying mechanisms provides a firm basis for investigations of multiscale air pollution and the nitrogen cycle

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