According to the particle size and absorptivity as determined by the fine mode fraction and the single-scattering albedo (SSA) retrievals from AErosol RObotic NETwork (AERONET) sites around the world, aerosols are classified into four key categories: coarse and absorptive aerosol (Type I), mixed aerosol (Type II), fine and absorptive aerosol (Type III), fine and non-absorptive aerosol (Type IV). Seasonal variations of aerosol types with their corresponding direct radiative forcing efficiency (RFE) are observed on different continents. The RFE at the surface (RFEsfc) and top of the atmosphere (RFEtoa) reach their maximum (minimum) values over Asia and North America (Europe, Oceania, and South America) from June to August. The effects of solar zenith angle (SZA), surface albedo (SA), and SSA on RFEsfc and RFEtoa are investigated. The absolute values of RFE at TOA of all types of aerosols are largest at cos(SZA) =0.3 to 0.4. The increased SA reduces the absolute value of RFE both at SFC and TOA for all types of aerosols, and when SA reaches a specific threshold, depending on the type of aerosol, the RFEtoa turns positive. RFEtoa increases while RFEsfc decreases with decreasing SSA. The RFEsfc of the four categories of aerosol varies slightly in the same SZA, SSA and SA conditions, while RFEtoa is aerosol type dependent. It is found that larger particles reflect more solar energy into space per optical depth, resulting in an enhanced cooling effect under similar SZA, SSA, and SA conditions.

We present the first box model simulation results aimed at identification of possible effects of the atmospheric photochemical evolution of the organic component of biomass burning (BB) aerosol on the aerosol radiative forcing (ARF) and its efficiency (ARFE). The simulations of the dynamics of the optical characteristics of the organic aerosol (OA) were performed using a simple parameterization developed within the volatility basis set framework and adapted to simulate the multiday BB aerosol evolution in idealized isolated smoke plumes from Siberian fires (without dilution). Our results indicate that the aerosol optical depth can be used as a good proxy for studying the effect of the OA evolution on the ARF, but variations in the scattering and absorbing properties of BB aerosol can also affect its radiative effects, as evidenced by variations in the ARFE. Changes in the single scattering albedo (SSA) and asymmetry factor, which occur as a result of the BB OA photochemical evolution, may either reduce or enhance the ARFE as a result of their competing effects, depending on the initial concentration OA, the ratio of black carbon to OA mass concentrations and the aerosol photochemical age in a complex way. Our simulation results also reveal that (1) the ARFE at the top of the atmosphere is not significantly affected by the OA oxidation processes compared to the ARFE at the bottom of the atmosphere, and (2) the dependence of ARFE in the atmospheric column and on the BB aerosol photochemical ages almost mirrors the corresponding dependence of SSA.

Ground reaching solar radiation flux was simulated using a 1-dimensional radiative transfer (SBDART) and a 3-dimensional regional climate (RegCM 4.4) model and their seasonality against simultaneous surface measurements carried out using a CNR4 net Radiometer over a sub-Himalayan foothill site of south-east Asia was assessed for the period from March 2013-January 2015. The model simulated incoming fluxes showed a very good correlation with the measured values with correlation coefficient R-2 similar to 0.97. The mean bias errors between these two varied from -40 W m(-2) to +7 W m(-2) with an overestimation of 2-3% by SBDART and an underestimation of 2-9% by RegCM. Collocated measurements of the optical parameters of aerosols indicated a reduction in atmospheric transmission path by similar to 20% due to aerosol load in the atmosphere when compared with the aerosol free atmospheric condition. Estimation of aerosol radiative forcing efficiency (ARFE) indicated that the presence of black carbon (BC, 10-15%) led to a surface dimming by -26.14 W m(-2) tau(-1) and a potential atmospheric forcing of + 43.04 W m(-2) tau(-1). BC alone is responsible for > 70% influence with a major role in building up of forcing efficiency of + 55.69 W m(-2) tau(-1) (composite) in the atmosphere. On the other hand, the scattering due to aerosols enhance the outgoing radiation at the top of the atmosphere (ARFE(TOA) similar to -12.60 W m(-2) omega(-1)), the absence of which would have resulted in ARFE(TOA) of similar to+16.91 W m(-2) tau(-1) (due to BC alone). As a result, similar to 3/4 of the radiation absorption in the atmosphere is ascribed to the presence of BC. This translated to an atmospheric heating rate of similar to 1.0 K day(-1), with similar to 0.3 K day(-1) heating over the elevated regions (2-4 km) of the atmosphere, especially during pre-monsoon season. Comparison of the satellite (MODIS) derived and ground based estimates of surface albedo showed seasonal difference in their magnitudes (R-2 similar to 0.98 during retreating monsoon and winter; similar to 0.65 during pre-monsoon and monsoon), indicating that the reliability of the satellite data for aerosol radiative forcing estimation is more during the retreating and winter seasons.