An aerosol dynamic model including such processes of nucleation, condensation/evaporation, coagulation, sedimentation, hygroscopic growth and dry and wet deposition coupled with the gas-phase chemistry of the California Institute of Technology model and the aqueous-phase chemistry of the Regional Acid Deposition Model together with meteorological outputs of the MM5 model in a grid of 60 x 60 km(2) has been used to estimate anthropogenic aerosols in East Asia (95-145E, 20-50N) for the period of 2-30 April 2001 in the ACE-Asia experimental period. During this period an Asian dust event has been observed from 10 to 13 and 24-26 April in the Korean peninsula. The estimated anthropogenic aerosols excluding the Asian dust are implemented to estimate radiative forcing at the surface, at the top of atmosphere (TOA) and atmospheric aerosol absorption in East Asia using the National Center for Atmospheric Research column radiation model of the community climate model. The results indicate that the area averaged column integrated anthropogenic aerosol concentration in East Asia is estimated to be about 20 mg m(-2), of which 46%, 29%, 20%, 4% and 1% are contributed by mixed type, inorganic (IOC), sea salt, organic carbon and black carbon aerosol, respectively. The daytime area mean direct shortwave radiative forcing at the surface is found to be about -5.9 W m(-2), of which IOC and the mixed type aerosol contribute about 95% whereas that at TOA is about -4.1 W m(-2), of which the IOC and the mixed type aerosol contribute more than 90%. Consequently the area mean atmospheric absorption due to anthropogenic aerosol layer in East Asia is about 1.8 W m(-2). The result clearly confirms the existence of a cooling effect (negative forcing) due to the direct effect of anthropogenic aerosols at the surface and TOA in East Asia. However, the atmosphere of the troposphere above the ground is slightly heated due to absorbing aerosol layers that are composed of black carbon and the mixed type aerosol. (C) 2004 Elsevier Ltd. All rights reserved.

Vertical profiles of aerosol size, composition, and hygroscopic behavior from Center for Interdisciplinary Remotely Piloted Aircraft Studies (CIRPAS) Twin Otter and National Oceanic and Atmospheric Administration R/V Ronald H. Brown observations are used to construct a generic optical model of the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) aerosol. The model accounts for sulfate, black carbon, organic carbon, sea salt, and mineral dust. The effects of relative humidity and mixing assumptions (internal versus external, coating of dust by pollutants) are explicitly accounted for. The aerosol model is integrated with a Monte Carlo radiative transfer model to compute direct radiative forcing in the solar spectrum. The predicted regional average surface aerosol forcing efficiency (change in clear-sky radiative flux per unit aerosol optical depth at 500 nm) during the ACE-Asia intensive period is -65 Wm(-2) for pure dust and -60 Wm(-2) for pure pollution aerosol (clear skies). A three-dimensional atmospheric chemical transport model (Chemical Weather Forecast System (CFORS)) is used with the radiative transfer model to derive regional radiative forcing during ACE-Asia in clear and cloudy skies. Net regional solar direct radiative forcing during the 5-15 April 2001 dust storm period is -3 Wm(-2) at the top of the atmosphere and -17 Wm(-2) at the surface for the region from 20degreesN to 50degreesN and 100degreesE to 150degreesE when the effects of clouds on the direct forcing are included. The model fluxes and forcing efficiencies are found to be in good agreement with surface radiometric observations made aboard the R. H. Brown. Mean cloud conditions are found to moderate the top of atmosphere (TOA) radiative forcing by a factor of similar to3 compared to clear-sky calculations, but atmospheric absorption by aerosol is not strongly affected by clouds in this study. The regional aerosol effect at the TOA (climate forcing) of -3 Wm(-2) is comparable in magnitude, but of opposite sign, to present-day anthropogenic greenhouse gas forcing. The forcing observed during ACE-Asia is similar in character to that seen during other major field experiments downwind of industrial and biomass black carbon sources (e.g., the Indian Ocean Experiment (INDOEX)), insofar as the primary effect of aerosol is to redistribute solar heating from the surface to the atmosphere.

A three-dimensional aerosol transport-radiation model coupled with a general circulation model, Spectral Radiation-Transport Model for Aerosol Species (SPRINTARS), simulates atmospheric aerosol distributions and optical properties. The simulated results are compared with aerosol sampling and optical observations from ground, aircraft, and satellite acquired by intensive observation campaigns over east Asia in spring 2001. Temporal variations of the aerosol concentrations, optical thickness, and Angstrom exponent are in good agreement between the simulation and observations. The midrange values of the Angstrom exponent, even at the Asian dust storm events over the outflow regions, suggest that the contribution of the anthropogenic aerosol, such as carbonaceous and sulfate, to the total optical thickness is of an order comparable to that of the Asian dust. The radiative forcing by the aerosol direct and indirect effects is also calculated. The negative direct radiative forcing is simulated to be over -10 W m(-2) at the tropopause in the air mass during the large-scale dust storm, to which both anthropogenic aerosols and Asian dust contribute almost equivalently. The direct radiative forcing, however, largely depends on the cloud water content and the vertical profiles of aerosol and cloud. The simulation shows that not only sulfate and sea salt aerosols but also black carbon and soil dust aerosols, which absorb solar and thermal radiation, make strong negative radiative forcing by the direct effect at the surface, which may exceed the positive forcing by anthropogenic greenhouse gases over the east Asian region.

[1] Airborne levels of carbonaceous aerosols were measured using the Twin Otter aircraft during the Aerosol Characterization Experiment (ACE)-Asia. Particles were collected using a newly developed honeycomb denuder sampler and organic carbon (OC), elemental carbon (EC), and carbonate (CC) carbon levels determined using a thermal-optical carbon analyzer. During some flights, atmospheric layers could be identified as marine boundary, pollution dominated, or mineral dust dominated. Angstrom exponent ((a) over circle) values, calculated based on data from an onboard three-wavelength nephelometer, were used to discern the nature of some individual layers. Values of (a) over circle for individual layers ranged from 0.2 to 2, corresponding to dust- and pollution-dominated layers, respectively. OC and EC concentrations below 3 km ranged from 0.58 to 29 mug C m(-3) and from 0.20 to 1.8 mug C m 3, respectively. In general, for a given type of atmospheric layer, higher levels of total carbon (TC) were observed during ACE-Asia than those observed during ACE-2, Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) and Indian Ocean Experiment (INDOEX). Mixed layers of dust and pollution were found on some occasions. CC was detected in samples taken from layers in which (a) over circle = 1.6, indicating that significant amounts of dust can be present even though (a) over circle > 0.2. A linear regression of light absorption coefficient sigma(ap) (Mm(-1)) versus EC concentration had an r(2) of only 0.50, indicating that parameters other than the mass of EC significantly affected the value of sigma(ap). The mass absorption coefficient E-abs (m(2) g(-1)) varied by as much as a factor of 8 between sampling events, and the average value of 11 m(2) g(-1) (+/-5.0) agrees well with previous published values.