Atmospheric aerosols have important impacts on global radiative forcing, air pollution, and human health. This study investigated the optical and physical properties of aerosol layers over Australia from 2007 to 2019 using the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) Level 2 aerosol products. Australia was divided into three sub-regions (western highlands, central plains, and eastern ranges). Interannual and seasonal optical property variations in aerosol layers in the three sub-regions were analyzed and compared. Results showed that annual mean values of AOD(L) (lowest aerosol layer AOD) and AOD(T) (total AOD of all aerosol layers) were always higher in the eastern ranges region than the other two regions from 2007 to 2019. The reason could be that Australian population was predominantly located in the eastern ranges region, where more human activities could bring significant aerosol loadings. B-L (base height of the lowest aerosol layer), H-L (top height of the lowest aerosol layer), and H-H (top height of the highest aerosol layer) all showed trends of western highlands > eastern mountains > central plains, indicating that the higher the elevation, the higher the B-L, H-L, and H-H. T-L (thickness of the lowest aerosol layer) was higher during the day than at night, which might account for increased diurnal atmospheric convection and nocturnal aerosol deposition. DRL (depolarization ratio of the lowest aerosol layer) was higher in the western highlands and central plains than the eastern mountains, probably because these two regions have large deserts with more irregularly shaped dust aerosols. CRL (color ratio of the lowest aerosol layer) had slightly higher values in the eastern ranges than the other two regions, probably due to the wet climate of the eastern ranges, where aerosols were more hygroscopic and had larger particle sizes. This study can provide technical support for the control and management of regional air pollutants.

Aerosols with different vertical distribution and various optical properties induce diverse heating rates and thereby affecting convective boundary layer (CBL) development. Our results showed consistent CBL-suppression of aerosols during daytime with numerical experiments, in which aerosols were specified at different heights with synthesized single scattering albedo from 64 studies and asymmetry factor from 20 studies globally. Absorbing aerosols concentrated below but close to the CBL top had the strongest suppression effect on CBL development relative to that concentrated near surface or above CBL. Aerosol cooling effect by attenuating incident solar radiation and surface heat flux exceeded its warming effect by reheating the atmosphere layer with absorbed shortwave radiation, and eventually declined net heating rate, which inhibited CBL development, lowered mixed-layer potential temperature and stabilized atmospheric stratification. Stove effect of absorbing aerosols (CBL enhancement) under a zero background aerosol extinction coefficient is negligible for dominant dome effect (CBL suppression) which consistently suppresses CBL development regardless of aerosol vertical height and background aerosol extinction coefficient. Our study also highlighted the importance of specifying background aerosol extinction coefficient in numerical experiments for accurate assessment of aerosol radiative forcing and CBL-aerosol interactions.

As an important fraction of light-absorbing particles, black carbon (BC) has a significant warming effect, despite accounting for a small proportion of total aerosols. A comprehensive investigation was conducted on the characteristics of atmospheric aerosols and BC particles over Wuhan, China. Mass concentration, optical properties, and radiative forcing of total aerosols and BC were estimated using multi-source observation data. Results showed that the BC concentration monthly mean varied from 2.19 to 5.33 mu g m(-3). The BC aerosol optical depth (AOD) maximum monthly mean (0.026) occurred in winter, whereas the maximum total AOD (1.75) occurred in summer. Under polluted-air conditions, both aerosol radiative forcing (ARF) and BC radiative forcing (BCRF) at the bottom of the atmosphere (BOA) were strongest in summer, with values of -83.01 and -11.22 W m(-2), respectively. In summer, ARF at BOA on polluted-air days was more than two-fold that on clean-air days. In addition, compared with clean-air days, BCRF at BOA on polluted-air days was increased by 76% and 73% in summer and winter, respectively. The results indicate an important influence of particulate air pollution on ARF and BCRF. Furthermore, the average contribution of BCRF to ARF was 13.8%, even though the proportion of BC in PM2.5 was only 5.1%.

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.

Soot particles positively influence radiative forcing due to their strong absorption. Because of their chain-like structure, aggregated soot particles become more compact with the aging process, and the monomers or particles are always covered by water coatings. The optical parameters of two typical soot-water mixtures (i.e., an aggregate with core-shell monomers and a soot aggregate inside a water droplet) at 550 nm were investigated using the superposition T-matrix method, with a focus on the impact of the morphology and water coating of soot aggregates. For the soot aggregate with core-shell monomers, a relationship among the fractal dimension, relative humidity (RH) and monomer number was established and used to calculate optical parameters. The intensity of forward scattering declined with the increasing RH. The Cext, Csca, Cabs and SSA are much more insensitive to RH under higher RH conditions (RH > 90%) than at a lower RH level. In addition, hygroscopic shrinkage and the thickness of water coating have stronger effects on the optical properties of larger aggregated soot at higher RH than lower RH. For another mixing state, the soot aggregate inside a water droplet, the morphology of the soot core plays an important role in the optical properties when the thickness of the water shell is small. When the diameter ratio of the water droplet to the aggregated soot (D_ratio) changes from 1.2 to 2.8, Cext difference increases from 0.23 mu m(2) to 2.36 mu m(2) for particles with N = 100 and 500, whereas the SSA difference decreases from 0.12 to 0.01. If the agglomerated structure of the soot core is not considered, the Cext, Csca and SSA will be underestimated for a relatively small D_ratio of 1.2. Ignoring the soot core in the water droplet could introduce large errors into the calculation of the optical parameters, and ignoring the structure of the aggregated soot core could enlarge the errors.

In this study, the influences of water solubility and light absorption on the optical properties of organic aerosols were investigated. A size-resolved model for calculating optical properties was developed by combining thermodynamic hygroscopic growth and aerosol dynamics models. The internal mixtures based on the homogeneous and core shell mixing were compared. The results showed that the radiative forcing (RF) of Water Soluble Organic Carbon (WSOC) aerosol can be estimated to range from -0.07 to -0.49 W/m(2) for core shell mixing and from -0.09 to -0.47 W/m(2) for homogeneous mixing under the simulation conditions (RH = 60%). The light absorption properties of WSOC showed the mass absorption efficiency (MAE) of WSOC can be estimated 0.43-0.5 m(2)/g, which accounts for 5-10% of the MAE of elemental carbon (EC). The effect on MAE of increasing the imaginary refractive index of WSOC was also calculated, and it was found that increasing the imaginary refractive index by 0.001i enhanced WSOC aerosol absorption by approximately 0.02 m(2)/g. Finally, the sensitivity test results revealed that changes in the fine mode fraction (FMF) and in the geometric mean diameter of the acthmulation mode play important roles in estimating RF during hygroscopic growth. (C) 2015 Elsevier Ltd. All rights reserved.