Assessment of Individual Direct Radiative Effects of Major Aerosol Species in East Asia

To assess individual direct radiative effects of diverse aerosol species on a regional scale,the air quality modeling system RAMS-CMAQ(Regional Atmospheric Modeling System and Community Multiscale Air Quality) coupled with an aerosol optical properties/radiative transfer module was used to simulate the temporal and spatial distributions of their optical and radiative properties over East Asia throughout 2005.Annual and seasonal averaged aerosol direct radiative forcing(ADRF) of all important aerosols and individual components,such as sulfate,nitrate,ammonium,black carbon(BC),organic carbon(OC),and dust at top-of-atmosphere(TOA) in clear sky are analyzed.Analysis of the model results shows that the annual average ADRF of all important aerosols was in the range of 0 to-18 W m?2,with the maximum values mainly distributed over the Sichuan Basin.The direct radiative effects of sulfate,nitrate,and ammonium make up most of the total ADRF in East Asia,being concentrated mainly over North and Southeast China.The model domain is also divided into seven regions based on different administrative regions or countries to investigate detailed information about regional ADRF variations over East Asia.The model results show that the ADRFs of sulfate,ammonium,BC,and OC were stronger in summer and weaker in winter over most regions of East Asia,except over Southeast Asia.The seasonal variation in the ADRF of nitrate exhibited the opposite trend.A strong ADRF of dust mainly appeared in spring over Northwest China and Mongolia.     

The impacts of optical properties on radiative forcing due to dust aerosol

There are large uncertainties in the quantitative assessment of radiative effects due to atmospheric dust aerosol. The optical properties contribute much to those uncertainties. The authors perform several sensitivity experiments to estimate the impacts of optical characteristics on regional radiative forcing in this paper. The experiments involve in refractive indices, single scattering aibedo, asymmetry factor and optical depth. An updated dataset of refractive indices representing East Asian dust and the one recommended by the World Meteorology Organization （WMO） are contrastively analyzed and used. A radiative transfer code for solar and thermal infrared radiation with detailed aerosol parameterization is employed. The strongest emphasis is on the refractive indices since other optical parameters strongly depend on it, and the authors found a strong sensitivity of radiative forcing on refractive indices. Studies show stronger scattering, weaker absorption and forward scattering of the East Asian dust particles at solar wavelengths, which leads to higher negative forcing, lower positive forcing and bigger net forcing at the top of the atmosphere （TOA） than that of the WMO dust model. It is also found that the TOA forcings resulting from these two dust models have opposite signs in certain regions, which implies the importance of accurate measurements of optical properties in the quantitative estimation of radiative forcing.     

Aerosol optical properties and its radiative forcing over Yulin,China in 2001 and 2002

The aerosol optical properties and direct radiative forcing over the Mu Us desert of northern China, acquired through a CE318 sunphotometer of the ground-based Aerosol Robotic Network (AERONET), are analyzed. The seasonal variations in the aerosol optical properties are examined. The effect of meteorological elements (pressure, temperature, water vapor pressure, relative humidity and wind speed) on the aerosol optical properties is also studied. Then, the sources and optical properties under two different cases, a dust event and a pollution event, are compared. The results show that the high aerosol optical depth (AOD) found in Yulin was mostly attributed to the occurrence of dust events in spring from the Mu Us desert and deserts of West China and Mongolia, as well as the impacts of anthropogenic pollutant particles from the middle part of China in the other seasons. The seasonal variation and the probability distribution of the radiative forcing and the radiative forcing efficiency at the surface and the top of the atmosphere are analyzed and regressed using the linear and Gaussian regression methods.     

Model Analysis of the Anthropogenic Aerosol Effect on Clouds over East Asia

A coupled meteorology and aerosol/chemistry model WRF-Chem(Weather Research and Forecast model coupled with Chemistry) was used to conduct a pair of simulations with present-day(PD) and preindustrial(PI) emissions over East Asia to examine the aerosol indirect effect on clouds.As a result of an increase in aerosols in January,the cloud droplet number increased by 650 cm-3 over the ocean and East China,400 cm-3 over Central and Southwest China,and less than 200 cm-3 over North China.The cloud liquid water path(LWP) increased by 40-60 g m-2 over the ocean and Southeast China and 30 g m-2 over Central China;the LWP increased less than 5 g m-2 or decreased by 5 g m-2 over North China.The effective radius(Re) decreased by more than 4 μm over Southwest,Central,and Southeast China and 2μm over North China.In July,variations in cloud properties were more uniform;the cloud droplet number increased by approximately 250-400 cm-3,the LWP increased by approximately 30-50 g m-2,and Re decreased by approximately 3 ?m over most regions of China.In response to cloud property changes from PI to PD,shortwave(SW) cloud radiative forcing strengthened by 30 W m-2 over the ocean and 10 W m-2 over Southeast China,and it weakened slightly by approximately 2-10 W m-2 over Central and Southwest China in January.In July,SW cloud radiative forcing strengthened by 15 W m-2 over Southeast and North China and weakened by 10 W m-2 over Central China.The different responses of SW cloud radiative forcing in different regions was related to cloud feedbacks and natural variability.     

Aerosol Direct Radiative Forcing over Shandong Peninsula in East Asia from 2004 to 2011

Recent vigorous industrialization and urbanization in Shandong Peninsula,China,have resulted in the emission of heavy anthropogenic aerosols over the region.The annual means of aerosol optical depth（AOD）,Angstrom exponent（α）,single-scattering albedo（SSA）,aerosol direct radiative forcing（ARF）,surface radiative forcing（SRF）,and top-of-the atmospheric radiative forcing（TOA） recorded during 2004–2011 were respectively 0.67±0.19,1.25±0.24,0.93±0.03,47±9 W m^-2,-61±9 W m^-2,and-14±8 W m^-2.The aerosol optical properties and ARF characteristics showed remarkable seasonal variations due to cycle changes in the aerosol components and dominance type.The atmosphere-surface system was cooled by ARF in all years of the study due to anthropogenic sulfate and nitrate emission and sea salt aerosols.The magnitude of TOA cooling was larger in summer（-15±17 W m^-2） and autumn（-12±7 W m^-2） than that in spring（-8±4 W m^-2） and winter（-9±10 W m^-2）.     

Development of RAMS-CMAQ to Simulate Aerosol Optical Depth and Aerosol Direct Radiative Forcing and Its Application to East Asia

The air quality modeling system RAMS （Regional Atmospheric Modeling System）-CMAQ （Models-3 Community Multi-scale Air Quality） is developed to simulate the aerosol optical depth （AOD） and aerosol direct forcing （DF）. The aerosol-specific extinction, single scattering albedo, and asymmetry factor are parameterized based on Mie theory taking into account the aerosol size distribution, composition, refractive index, and water uptake of solution particles. A two-stream solar radiative model considers all gaseous molecular absorption, Rayleigh scattering, and aerosols and clouds. RAMSCMAQ is applied to simulate all major aerosol concentrations （e.g., sulfate, nitrate, ammonium, organic carbon, black carbon, fine soil, and sea salt） and AOD and DF over East Asia in 2005. To evaluate its performance, the simulated AOD values were compared with ground-based in situ measurements. The comparison shows that RAMSCMAQ performed well in most of the model domain and generally captured the observed variations. High AOD values （0.2-1.0） mainly appear in the Sichuan Basin as well as in central and southeastern China. The geographic distribution of DF generally follows the AOD distribution patterns, and the DF at the top-of-the-atmosphere is less than -25 and -20 W m^-2 in clear-sky and all-sky over the Sichuan Basin. Both AOD and DF exhibit seasonal variations with lower values in July and higher ones in January. The DF could obviously be impacted by high cloud fractions.     

基于AERONET的西亚地区气溶胶光学特性

利用AERONET 10个站点的Level2数据分析得到2010-2017年西亚地区多个气溶胶参数(光学厚度(Aerosol Optical Depth,AOD)、吸收光学厚度(Absorption Aerosol Optical Depth,AAOD)、波长指数α、粒子体积谱和单次散射反照率(Single Scatt...     

Modeling Study of the Impact of Heterogeneous Reactions on Dust Surfaces on Aerosol Optical Depth and Direct Radiative Forcing over East Asia in Springtime

The spatial distributions and interannual variations of aerosol concentrations,aerosol optical depth(AOD) ,aerosol direct radiative forcings,and their responses to heterogeneous reactions on dust surfaces over East Asia in March 2006-10 were investigated by utilizing a regional coupled climate-chemistry/aerosol model. Anthropogenic aerosol concentrations(inorganic+carbonaceous) were higher in March 2006 and 2008,whereas soil dust reached its highest levels in March 2006 and 2010,resulting in stronger aerosol radiative forcings in these periods.The domain and five-year(2006-10) monthly mean concentrations of anthropogenic and dust aerosols,AOD,and radiative forcings at the surface(SURF) and at the top of the atmosphere(TOA) in March were 2.4μg m-3,13.1μg m-3,0.18,-19.0 W m-2,and-7.4 W m-2,respectively.Heterogeneous reactions led to an increase of total inorganic aerosol concentration;however,the ambient inorganic aerosol concentration decreased,resulting in a smaller AOD and weaker aerosol radiative forcings.In March 2006 and 2010,the changes in ambient inorganic aerosols,AOD,and aerosol radiative forcings were more evident.In terms of the domain and five-year averages,the total inorganic aerosol concentrations increased by 13.7%(0.17μg m-3) due to heterogeneous reactions,but the ambient inorganic aerosol concentrations were reduced by 10.5%(0.13μg m-3) .As a result,the changes in AOD,SURF and TOA radiative forcings were estimated to be-3.9%(-0.007) ,-1.7%(0.34 W m-2) ,and-4.3%(0.34 W m-2) ,respectively,in March over East Asia.     

CFMIP大气环流模式模拟的东亚云辐射强迫特征

通过与卫星观测云和辐射资料的比较,检验了10个大气环流模式对东亚地区云量、垂直结构、光学属性以及辐射特征的模拟能力.10个模式的模拟结果均来自"云反馈模式比较计划"(CFMIP),为便于与国际卫星云气候计划(ISCCP)资料的比较,所有模式都引入了ISCCP模拟器.结果表明,10个模式均能模拟出东亚地区冬、夏两季云量及...     

Optical,Radiative and Chemical Characteristics of Aerosol in Changsha City,Central China

Industrial pollution has a significant effect on aerosol properties in Changsha City, a typical city of central China.Therefore, year-round measurements of aerosol optical, radiative and chemical properties from 2012 to 2014 at an urban site in Changsha were analyzed. During the observation period, the energy structure was continuously optimized, which was characterized by the reduction of coal combustion. The aerosol properties have obvious seasonal variations. The seasonal average aerosol opti...     

东亚沙尘源区与下游地区气溶胶光学特性比较

利用AERONET观测资料从气候学的角度比较分析了2001-2011年东亚地区沙尘天气发生时沙尘源区和下游区大气气溶胶光学特性。结果表明：沙尘期间沙尘源区气溶胶光学厚度明显大于下游区,而Angstr?m波长指数却小于下游区,当沙尘暴出现时会降至零甚至负值。气溶胶粒子尺度体积谱分布除敦煌为单峰外,其余各站均呈双峰分布,香河和北京的细粒子浓度明显大于西北地区,这可能是由细的沙尘粒子和污染气溶胶共同造成。在440-1020 nm范围内,中国地区气溶胶单次散射反照率平均值为0.93,韩国和日本站分别为0.93和0.94。沙尘源区与下游区相比,复折射指数实部偏大,虚部偏小。总体来说,沙尘天气下东亚地区在4个波段内平均不对称因子为0.70。     

Direct Climatic Effect of Dust Aerosol in the NCAR Community Atmosphere Model Version 3 （CAM3）

Direct climate responses to dust shortwave and longwave radiative forcing (RF) are studied using the NCAR Community Atmosphere Model Version 3 (CAM3). The simulated RF at the top of the atmosphere (TOA) is-0.45 W m-2 in the solar spectrum and +0.09 W m-2 in the thermal spectrum on a global average. The magnitude of surface RF is larger than the TOA forcing, with global mean shortwave forcing of-1.76 W m-2 and longwave forcing of +0.31 W m-2 . As a result, dust aerosol causes the absorption of 1.1 W m-2 in t...     

Effect of particle shape on dust shortwave direct radiative forcing calculations based on MODIS observations for a case study

Assuming spheroidal and spherical particle shapes for mineral dust aerosols, the effect of particle shape on dust aerosol optical depth retrievals, and subsequently on instantaneous shortwave direct radiative forcing (SWDRF) at the top of the atmosphere (TOA), is assessed based on Moderate Resolution Imaging Spectroradiometer (MODIS) data for a case study. Specifically, a simplified aerosol retrieval algorithm based on the principle of the Deep Blue aerosol retrieval method is employed to retrieve dust aerosol optical depths, and the Fu-Liou radiative transfer model is used to derive the instantaneous SWDRF of dust at the TOA for cloud-free conditions. Without considering the effect of particle shape on dust aerosol optical depth retrievals, the effect of particle shape on the scattering properties of dust aerosols (e.g., extinction efficiency, single scattering albedo and asymmetry factor) is negligible, which can lead to a relative difference of at most 5% for the SWDRF at the TOA. However, the effect of particle shape on the SWDRF cannot be neglected provided that the effect of particle shape on dust aerosol optical depth retrievals is also taken into account for SWDRF calculations. The corresponding results in an instantaneous case study show that the relative differences of the SWDRF at the TOA between spheroids and spheres depend critically on the scattering angles at which dust aerosol optical depths are retrieved, and can be up to 40% for low dust-loading conditions.     

Direct Radiative Forcing and Climatic Effects of Aerosols over East Asia by RegCM3

The authors used a high-resolution regional climate model(RegCM3) coupled with a chemistry/aerosol module to simulate East Asian climate in 2006 and to test the climatic impacts of aerosols on regionalscale climate.The direct radiative forcing and climatic effects of aerosols(dust,sulfate,black carbon,and organic carbon) were discussed.The results indicated that aerosols generally produced negative radiative forcing at the top-of-the-atmosphere(TOA) over most areas of East Asia.The radiative forcing induced by aerosols exhibited significant seasonal and regional variations,with the strongest forcing occurring in summer.The aerosol feedbacks on surface air temperature and precipitation were clear.Surface cooling dominated features over the East Asian continental areas,which varied in the approximate range of-0.5 to-2°C with the maximum up to-3-C in summer over the deserts of West China.The aerosols induced complicated variations of precipitation.Except in summer,the rainfall generally varied in the range of-1 to 1 mm d-1 over most areas of China.     

A Study on Sulfate Optical Properties and Direct Radiative Forcing Using LASG-IAP General Circulation Model

The direct radiative forcing(DRF) of sulfate aerosols depends highly on the atmospheric sulfate loading and the meteorology,both of which undergo strong regional and seasonal variations.Because the optical properties of sulfate aerosols are also sensitive to atmospheric relative humidity,in this study we first examine the scheme for optical properties that considers hydroscopic growth.Next,we investigate the seasonal and regional distributions of sulfate DRF using the sulfate loading simulated from NCAR CAM-Chem together with the meteorology modeled from a spectral atmospheric general circulation model(AGCM) developed by LASG-IAP.The global annual-mean sulfate loading of 3.44 mg m 2 is calculated to yield the DRF of 1.03 and 0.57 W m 2 for clear-sky and all-sky conditions,respectively.However,much larger values occur on regional bases.For example,the maximum all-sky sulfate DRF over Europe,East Asia,and North America can be up to 4.0 W m 2.The strongest all-sky sulfate DRF occurs in the Northern Hemispheric July,with a hemispheric average of 1.26 W m 2.The study results also indicate that the regional DRF are strongly affected by cloud and relative humidity,which vary considerably among the regions during different seasons.This certainly raises the issue that the biases in model-simulated regional meteorology can introduce biases into the sulfate DRF.Hence,the model processes associated with atmospheric humidity and cloud physics should be modified in great depth to improve the simulations of the LASG-IAP AGCM and to reduce the uncertainty of sulfate direct effects on global and regional climate in these simulations.     

Comparison of column-integrated aerosol optical and physical properties in an urban and suburban site on the North China Plain

The column-integrated optical properties of aerosol in Beijing and Xianghe, two AErosol RObotic NETwork(AERONET)sites situated on the North China Plain(NCP), are investigated based on Cimel sunphotometer measurements from October2004 to June 2012. The outstanding feature found is that the seasonal medians of aerosol optical depth(AOD) at the two stations are in good agreement. The correlation coefficients and the absolute differences between AOD at the two stations are larger than 0.84 and less than 0.05, respectively. Good agreement in AOD at these two sites(one urban and the other suburban; 70 km apart) indicates that aerosol pollution in the Greater Beijing area is regional in nature. However, we find significant differences in the absorption ?Angstr ¨om Exponent(AAE), the real and imaginary part of the refractive index, and thereby the single scattering albedo(SSA), and the difference is seasonally dependent. The feature is found to be more prominent in fall when the fine-mode fraction(FMF) and fine-mode effective radius are significantly different at the two stations,besides the parameters mentioned above. The SSA in Beijing at four wavelengths shows lower values as compared to those in Xianghe, although the difference is not significant in some cases. Significant differences in AAE and fine-mode effective radius indicate that there are differences in aerosol physical and chemical properties in urban and suburban regions on the NCP.     

Grid-cell Aerosol Direct Shortwave Radiative Forcing Calculated Using the SBDART Model with MODIS and AERONET Observations:An Application in Winter and Summer in Eastern China

Taking winter and summer in eastern China as an example application, a grid-cell method of aerosol direct radiative forcing(ADRF) calculation is examined using the Santa Barbara DISORT Atmospheric Radiative Transfer(SBDART) model with inputs from MODIS and AERONET observations and reanalysis data. Results show that there are significant seasonal and regional differences in climatological mean aerosol optical parameters and ADRF. Higher aerosol optical depth(AOD)occurs in summer and two prominent high aerosol loading centers are observed. Higher single scattering albedo(SSA) in summer is likely associated with the weak absorbing secondary aerosols. SSA is higher in North China during summer but higher in South China during winter. Aerosols induce negative forcing at the top of the atmosphere(TOA) and surface during both winter and summer, which may be responsible for the decrease in temperature and the increase in relative humidity.Values of ADRF at the surface are four times stronger than those at the TOA. Both AOD and ADRF present strong interannual variations; however, their amplitudes are larger in summer. Moreover, patterns and trends of ADRF do not always correspond well to those of AOD. Differences in the spatial distributions of ADRF between strong and weak monsoon years are captured effectively. Generally, the present results justify that to calculate grid-cell ADRF at a large scale using the SBDART model with observational aerosol optical properties and reanalysis data is an effective approach.     

A Modeling Study of the Effects of Direct Radiative Forcing Due to Carbonaceous Aerosol on the Climate in East Asia

The study investigated the effects of global direct radiative forcing due to carbonaceous aerosol on the climate in East Asia, using the CAM3 developed by NCAR. The results showed that carbonaceous aerosols cause negative forcing at the top of the atmosphere (TOA) and surface under clear sky conditions, but positive forcing at the TOA and weak negative forcing at the surface under all sky conditions. Hence, clouds could change the sign of the direct radiative forcing at the TOA, and weaken the forcing at the surface. Carbonaceous aerosols have distinct effects on the summer climate in East Asia. In southern China and India, it caused the surface temperature to increase, but the total cloud cover and precipitation to decrease. However, the opposite effects are caused for most of northern China and Bangladesh. Given the changes in temperature, vertical velocity, and surface streamflow caused by carbonaceous aerosol in this simulation, carbonaceous aerosol could also induce summer precipitation to decrease in southern China but increase in northern China.     

Direct Climatic Effect of Aerosols and Interdecadal Variations over East Asia Investigated by a Regional Coupled Climate-chemistry/aerosol Model

The direct climatic effect of aerosols for the 1980-2000 period over East Asia was numerically investigated by a regional scale coupled climate-chemistry/aerosol model,which includes major anthropogenic aerosols(sulfate,black carbon,and organic carbon) and natural aerosols(soil dust and sea salt) .Anthropogenic emissions used in model simulation are from a global emission inventory prepared for the Intergovernmental Panel on Climate Change Fifth Assessment Report(IPCC AR5) ,whereas natural aerosols are calculated online in the model.The simulated 20-year average direct solar radiative effect due to aerosols at the surface was estimated to be in a range of-9--33 W m-2 over most areas of China,with maxima over the Gobi desert of West China,and-12 W m-2 to-24 W m-2 over the Sichuan Basin,the middle and lower reaches of the Yellow River and the Yangtze River.Aerosols caused surface cooling in most areas of East Asia,with maxima of-0.8-C to-1.6-C over the deserts of West China,the Sichuan Basin,portions of central China,and the middle reaches of the Yangtze River. Aerosols induced a precipitation decrease over almost the entire East China,with maxima of-90 mm/year to-150 mm/year over the Sichuan Basin,the middle reaches of the Yangtze River and the lower reaches of the Yellow River.Interdecadal variation of the climate response to the aerosol direct radiative effect is evident,indicating larger decrease in surface air temperature and stronger perturbation to precipitation in the 1990s than that in the 1980s,which could be due to the interdecadal variation of anthropogenic emissions.     

One year measurements of aerosol optical properties over an urban coastal site: Effect on local direct radiative forcing

We present results of direct aerosol radiative forcing over a French Mediterranean coastal zone based on one year of continuous observations of aerosol optical properties during 2005–2006. Monthly-mean aerosol optical depth at 440 nm ranged between 0.1 and 0.34, with high Angstrom coefficient (α > 1.2). The single scattering albedo (at 525 nm) estimated at the surface ranged between 0.7 and 0.8, indicating significant absorption. The presence of aerosols over the Mediterranean zone during summer decreases the shortwave radiation reaching the surface by as much as 26 ± 3.9 W m^− 2, and increases the top of the atmosphere reflected radiation by as much as 5.2 ± 1.0 W m^− 2. The shortwave atmospheric absorption translates to an atmospheric heating of 2.5 to 4.6 K day^− 1. Concerted efforts are needed for investigating the possible impact of the increase in heating rate on the maintenance of heat-waves frequently occurring over this coastal region during summer time.