Abstract

Abstract. To more accurately estimate direct radiative forcing (DRF) by aerosols, and better investigate particulate pollution over East Asia, precise calculations of the optical properties of aerosols, such as aerosol optical depth (AOD), single scattering albedo (SSA) and aerosol extinction coefficient (σext), are of primary importance. The aerosol optical properties over East Asia were investigated in this study, based on US EPA Models-3/CMAQ v4.5.1 model simulations. The CMAQ model simulations in this study were improved in several ways compared to those in a previous study (Song et al., 2008). Although the details of the improvements were described in the manuscript, the following points should be emphasized: (1) two data assimilation techniques were employed for producing more accurate AOD products and meteorological fields over East Asia; (2) updated/upgraded emission inventories were used in the CMAQ model simulations with a fine grid resolution of 30 × 30 km2; and (3) the 4-D particulate composition calculated from the CMAQ model simulations was converted into 3-D or 4-D aerosol optical products, using the Malm and Hand (2007) algorithm with significant further modifications. The results from the CMAQ model simulations (without assimilation) showed great improvements compared to those from a previous study. For example, in terms of the regression coefficients (R), R values were increased from 0.48–0.68 (previous study) to 0.62–0.79 (this study). The monthly-averaged CMAQ-simulated single scattering albedo (SSA) also agreed well with the AERONET SSA, with the exceptions of the Hong Kong and Taipei sites, where the air qualities were strongly influenced by active biomass burning events from January to April. There were also excellent matches between the vertical profiles of the CMAQ-simulated σext and LIDAR-retrieved σext. It was also found that the contributions of (NH4)2SO4 during summer, NH4NO3 during winter, sea-salt particles during winter and dust particles during spring to the total AOD were large over East Asia. In particular, the largest contribution of NH4NO3 to the total AOD was found over East Asia during winter. Therefore, it was suggested that this contribution of NH4NO3 should not be neglected. In order to produce more accurate AOD products, the CMAQ-simulated AODs were further assimilated with the MODIS-retrieved AODs. Both of the assimilated and AERONET AODs were better correlated with each other than the CMAQ-simulated and AERONET AODs. The obvious benefits from this study would be that with these improved aerosol optical properties, the particulate pollution (e.g. AOD can be served as a proxy to PM2.5 or PM10) and DRF by aerosols over East Asia can be more satisfactorily investigated in future.

Highlights

  • The importance of the roles of aerosols in global climate change and particulate pollution has been discussed for several decades

  • As reported by Bian et al (2009), the high spatial and temporal resolutions used in the MM5-CMAQ model simulations can further enhance the accuracy of the aerosol optical depth (AOD) products, since the relative humidity fields frequently exhibit high heterogeneities in both space and time

  • 4-D aerosol optical products, using the Malm and Hand (2007) algorithm with further modifications; and (8) the CMAQ-simulated AOD products were assimilated with the MODIS-retrieved AOD, using the optimal interpolation technique

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Summary

Introduction

The importance of the roles of aerosols in global climate change and particulate pollution has been discussed for several decades. The aerosol optical depth (AOD) is empirically well-correlated with PM2.5 and/or PM10; the ratios of the AOD to particulate concentrations have been used to estimate the spatial distributions of PM2.5 and/or PM10 at surface levels To better understand and investigate atmospheric aerosols in East Asia, several research campaigns have been conducted in East Asia, including ground-based monitoring, aircraft and ship measurements (e.g. PEM-West A and B, ACE-Asia, and TRACEP). Such field campaigns have been limited by an inability to completely cover the spatial and temporal variations of aerosol concentrations and aerosol optical properties

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