We extend a stochastic aerosol-snow albedo model to explicitly simulate dust internally/externally mixed with snow grains of different shapes and for the first time quantify the combined effects of dust-snow internal mixing and snow nonsphericity on snow optical properties and albedo. Dust-snow internal/external mixing significantly enhances snow single-scattering coalbedo and absorption at wavelengths of <1.0 mu m, with stronger enhancements for internal mixing (relative to external mixing) and higher dust concentrations but very weak dependence on snow size and shape variabilities. Compared with pure snow, dust-snow internal mixing reduces snow albedo substantially at wavelengths of <1.0 mu m, with stronger reductions for higher dust concentrations, larger snow sizes, and spherical (relative to nonspherical) snow shapes. Compared to internal mixing, dust-snow external mixing generally shows similar spectral patterns of albedo reductions and effects of snow size and shape. However, relative to external mixing, dust-snow internal mixing enhances the magnitude of albedo reductions by 10%-30% (10%-230%) at the visible (near-infrared) band. This relative enhancement is stronger as snow grains become larger or nonspherical, with comparable influences from snow size and shape. Moreover, for dust-snow external and internal mixing, nonspherical snow grains have up to similar to 45% weaker albedo reductions than spherical grains, depending on snow size, dust concentration, and wavelength. The interactive effect of dust-snow mixing state and snow shape highlights the importance of accounting for these two factors concurrently in snow modeling. For application to land/climate models, we develop parameterizations for dust effects on snow optical properties and albedo with high accuracy.

Influences of the mixing treatments of anthropogenic aerosols on their effective radiative forcing (ERF) and global aridity are evaluated by using the BCC_AGCM2.0_CUACE/Aero, an aerosol-climate online coupled model. Simulations show that the negative ERF due to external mixing (EM, a scheme in which all aerosol particles are treated as independent spheres formed by single substance) aerosols is largely reduced by the partial internal mixing (PIM, a scheme in which some of the aerosol particles are formed by one absorptive and one scattering substance) method. Compared to EM, PIM aerosols have much stronger absorptive ability and generally weaker hygroscopicity, which would lead to changes in radiative forcing, hence to climate. For the global mean values, the ERFs due to anthropogenic aerosols since the pre-industrial are-1.02 and-1.68 W m(-2) for PIM and EM schemes, respectively. The variables related to aridity such as global mean temperature, net radiation flux at the surface, and the potential evaporation capacity are all decreased by 2.18/1.61 K, 5.06/3.90 W m(-2), and 0.21/0.14 mm day(-1) since 1850 for EM and PIM schemes, respectively. According to the changes in aridity index, the anthropogenic aerosols have caused general humidification over central Asia, South America, Africa, and Australia, but great aridification over eastern China and the Tibetan Plateau since the pre-industrial in both mixing schemes. However, the aridification is considerably alleviated in China, but intensified in the Arabian Peninsula and East Africa in the PIM scheme.

We quantify the effects of grain shape and multiple black carbon (BC)-snow internal mixing on snow albedo by explicitly resolving shape and mixing structures. Nonspherical snow grains tend to have higher albedos than spheres with the same effective sizes, while the albedo difference due to shape effects increases with grain size, with up to 0.013 and 0.055 for effective radii of 1,000m at visible and near-infrared bands, respectively. BC-snow internal mixing reduces snow albedo at wavelengths < similar to 1.5m, with negligible effects at longer wavelengths. Nonspherical snow grains show less BC-induced albedo reductions than spheres with the same effective sizes by up to 0.06 at ultraviolet and visible bands. Compared with external mixing, internal mixing enhances snow albedo reduction by a factor of 1.2-2.0 at visible wavelengths depending on BC concentration and snow shape. The opposite effects on albedo reductions due to snow grain nonsphericity and BC-snow internal mixing point toward a careful investigation of these two factors simultaneously in climate modeling. We further develop parameterizations for snow albedo and its reduction by accounting for grain shape and BC-snow internal/external mixing. Combining the parameterizations with BC-in-snow measurements in China, North America, and the Arctic, we estimate that nonspherical snow grains reduce BC-induced albedo radiative effects by up to 50% compared with spherical grains. Moreover, BC-snow internal mixing enhances the albedo effects by up to 30% (130%) for spherical (nonspherical) grains relative to external mixing. The overall uncertainty induced by snow shape and BC-snow mixing state is about 21-32%. Plain Language Summary Pure snow strongly reflects sunlight, the degree of which is regulated by grain size and shape. Observations have shown that snow can be significantly darkened by impurities, such as black carbon (BC), which is the most important light-absorbing aerosol. However, the combined effects of the two critical factors, snow grain shape and BC-snow mixing structure, have not been previously investigated, the neglect of which could introduce large uncertainties in the estimates of snow albedo in terms of BC-induced darkening. We have developed a snow model to quantify the impact of the preceding two factors on snow albedo by means of resolving the structures of BC-snow mixtures for different grain shapes. Both snow grain shape and multiple BC-snow internal mixing play important roles in their impacts on snow albedo. For application to climate models, we construct a scheme to parameterize snow albedo and its darkening in terms of snow grain size, shape, and BC content.

A partial internal mixing (PIM) treatment of black carbon (BC), organic carbon (OC), and sulphate was examined, and the core-shell model was used to represent the internally mixed aerosols with BC as the core and sulphate or OC as the shell. The influences of PIM treatment on the effective radiative forcing due to aerosol-radiative interaction (ERFari) and global temperature were examined and compared to those of external mixing (EM) treatment using an aerosol-climate online coupled model of BCC_AGCM2.0_CUACE/Aero. Radiative forcing due to aerosol-radiation interaction (RFari) of the anthropogenic aerosols since the preindustrial era was -0.34 W m(-2) for EM and -0.23 W m(-2) for PIM, respectively. The global annual mean ERFari of anthropogenic aerosols since the preindustrial era was -0.42 W m(-2) for EM and -0.34 W m(-2) for PIM, respectively. The change in global annual mean surface temperature increased accordingly from -0.18K in the EM case to -0.125K in the PIM case. Well geographic consistence between the change in low-level cloud amount and the change in temperature can be found. The atmospheric temperature in the troposphere was markedly less reduced in the PIM case than in the EM case. The RFari/ERFari for 50% and 100% were -0.11/-0.07 and 0.13/0.14 W m(-2), respectively. RFari, ERFari, and surface temperature changed approximately linearly with the internal mixing proportion.

The air quality model system RAMS (Regional Atmospheric Modeling System)-CMAQ (Models-3 Community Multi-scale Air Quality) coupled with an aerosol optical/radiative module was applied to investigate the impact of different aerosol mixing states (i.e., externally mixed, half externally and half internally mixed, and internally mixed) on radiative forcing in East Asia. The simulation results show that the aerosol optical depth (AOD) generally increased when the aerosol mixing state changed from externally mixed to internally mixed, while the single scattering albedo (SSA) decreased. Therefore, the scattering and absorption properties of aerosols can be significantly affected by the change of aerosol mixing states. Comparison of simulated and observed SSAs at five AERONET (Aerosol Robotic Network) sites suggests that SSA could be better estimated by considering aerosol particles to be internally mixed. Model analysis indicates that the impact of aerosol mixing state upon aerosol direct radiative forcing (DRF) is complex. Generally, the cooling effect of aerosols over East Asia are enhanced in the northern part of East Asia (Northern China, Korean peninsula, and the surrounding area of Japan) and are reduced in the southern part of East Asia (Sichuan Basin and Southeast China) by internal mixing process, and the variation range can reach +/- 5 W m(-2). The analysis shows that the internal mixing between inorganic salt and dust is likely the main reason that the cooling effect strengthens. Conversely, the internal mixture of anthropogenic aerosols, including sulfate, nitrate, ammonium, black carbon, and organic carbon, could obviously weaken the cooling effect.

Optical properties of clouds containing black carbon (BC) particles in their water droplets are calculated by using the Maxwell Garnett mixing rule and Mie theory. The obtained cloud optical properties were then applied to an interactive system by coupling an aerosol model with a General Circulation Model. This system is used to investigate the radiative forcing and the equilibrium climate response due to BC in cloud droplets. The simulated global annual mean radiative forcing at the top of the atmosphere due to the BC in cloud droplets is found to be 0.086Wm-2. Positive radiative forcing can be seen in Africa, South America, East and South Asia, and West Europe, with a maximum value of 1.5Wm-2 being observed in these regions. The enhanced cloud absorption is shown to increase the global annual mean values of solar heating rate, water vapor, and temperature, but to decrease the global annual mean cloud fraction. Finally, the global annual mean surface temperature is shown to increase by +0.08K. The local maximum changes are found to be as low as -1.5K and as high as +0.6K. We show there has been a significant difference in surface temperature change in the Southern and Northern Hemisphere (+0.19K and -0.04K, respectively). Our results show that this interhemispheric asymmetry in surface temperature change could cause a corresponding change in atmospheric dynamics and precipitation. It is also found that the northern trade winds are enhanced in the Intertropical Convergence Zone (ITCZ). This results in northerly surface wind anomalies which cross the equator to converge with the enhanced southern trade winds in the tropics of Southern Hemisphere. This is shown to lead to an increase (a decrease) of vertical ascending motion and precipitation on the south (north) side of the equator, which could induce a southward shift in the tropical rainfall maximum related to the ITCZ.

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.