Abstract

Abstract. Anthropogenic SO2 emissions increased alongside economic development in China at a rate of 12.7% yr−1 from 2000 to 2005. However, under new Chinese government policy, SO2 emissions declined by 3.9% yr−1 between 2005 and 2009. Between 2000 and 2010, we found that the variability in the fine-mode (submicron) aerosol optical depth (AOD) over the oceans adjacent to East Asia increased by 3–8% yr−1 to a peak around 2005–2006 and subsequently decreased by 2–7% yr−1, based on observations by the Moderate Resolution Imaging Spectroradiometer (MODIS) on board NASA's Terra satellite and simulations by a chemical transport model. This trend is consistent with ground-based observations of aerosol particles at a mountainous background observation site in central Japan. These fluctuations in SO2 emission intensity and fine-mode AOD are thought to reflect the widespread installation of fuel-gas desulfurization (FGD) devices in power plants in China, because aerosol sulfate is a major determinant of the fine-mode AOD in East Asia. Using a chemical transport model, we confirmed that the contribution of particulate sulfate to the fine-mode AOD is more than 70% of the annual mean and that the abovementioned fluctuation in fine-mode AOD is caused mainly by changes in SO2 emission rather than by other factors such as varying meteorological conditions in East Asia. A strong correlation was also found between satellite-retrieved SO2 vertical column density and bottom-up SO2 emissions, both of which were also consistent with observed fine-mode AOD trends. We propose a simplified approach for evaluating changes in SO2 emissions in China, combining the use of modeled sensitivity coefficients that describe the variation of fine-mode AOD with changes in SO2 emissions and satellite retrieval. Satellite measurements of fine-mode AOD above the Sea of Japan marked a 4.1% yr−1 decline between 2007 and 2010, which corresponded to the 9% yr−1 decline in SO2 emissions from China during the same period.

Highlights

  • Atmospheric aerosols play an important role in the global energy budget and in modifying cloud properties, precipitation efficiency, and the characteristics of the atmospheric circulation

  • Between 2000 and 2010, we found that the variability in the fine-mode aerosol optical depth (AOD) over the oceans adjacent to East Asia increased by 3–8 % yr−1 to a peak around 2005–2006 and subsequently decreased by 2–7 % yr−1, based on observations by the Moderate Resolution Imaging Spectroradiometer (MODIS) on board NASA’s Terra satellite and simulations by a chemical transport model

  • We focused on the AODf over the oceans of the downwind region of central eastern China (CEC) in East Asia, and the modeled dominant contribution of sulfate is consistent with observation data from Korea and Japan (Carmichael et al, 1996; Osada et al, 2007)

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Summary

Introduction

Atmospheric aerosols play an important role in the global energy budget and in modifying cloud properties, precipitation efficiency, and the characteristics of the atmospheric circulation. Matsumoto et al (2003) reported that the mean concentrations of nss-SO24−, NO−3 , and NH+4 in aerosols were 2.48, 0.64, and 0.72 μg m−3, respectively, on Rishiri Island (45.07◦ N, 141.12◦ E), Japan, from March to May 2001 These aerosol measurements indicated that anthropogenic sulfate aerosols are a dominant contributor to the aerosol component in East Asia. From 2000 to 2005, anthropogenic SO2 emissions from China increased at a rate of 12.7 % yr−1 from 28 to 51 Mt yr−1 (Ohara et al, 2007) In this situation, the AOD increased over East Asia from 1980 to 2006, as shown by a global model and observed surface solar radiation (Streets et al, 2009). To understand the recent trend in fine-mode AOD and its relationship to the changes in anthropogenic emissions in East Asia, this study analyzed the trend in fine-mode AOD between 2000 and 2010 using emission inventory data with a bottom-up approach, space-based observations, and the results of a chemical transport model simulation

Satellite measurements and ground observation
Chemical transport model
Trends in AODf during 2000–2010
Conclusions
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