Shortcomings and uncertainties in the model representation of atmospheric transformations (the aging) of organic aerosol (OA) have long been identified as one of the potential sources of considerable uncertainty in OA simulations with both global and regional models. However, the impact of this uncertainty on predictions of radiative and climate effects of both anthropogenic and biomass burning (BB) aerosol yet needs to be understood. This study examines the importance of the model representation of OA for simulating the direct radiative effect (DRE) of Siberian BB aerosol in the eastern Arctic. We employ a regional coupled chemistry-meteorology model and a global fire emission database to simulate the optical properties and DRE of BB aerosol emitted from intense Siberian fires in July 2016 and compare the DRE estimates that were obtained using two alternative representations of Siberian BB OA. One of them is a default OA representation that predicts very little secondary OA (SOA), and another involves a simple original OA parameterization that has been developed previously within the volatility basis set (VBS) framework and features a strong production of SOA. The simulations of the aerosol optical properties are evaluated against satellite observations of the aerosol optical depth (AOD) in Siberia and the Arctic as well as against values of the single scattering albedo derived from in situ observations of the aerosol absorption and scattering coefficients at four Arctic sites. While the simulations with the default OA representation are found to strongly underestimate AOD both in Siberia and the eastern Arctic, the use of the VBS parameterization considerably improves the agreement between the AOD simulations and observations in both regions. Simulations of the single scattering albedo are found to be overall rather adequate with both representations. Differences in the OA representations are found to result in major differences in the estimates of the DRE of Siberian BB aerosol in the eastern Arctic. Specifically, although the simulations with both representations predict that the DRE is predominantly negative at the top of the atmosphere (TOA), the magnitude of the mean DRE is found to be more than twice as large (6.0 W m-2) with the VBS parameterization than with the default OA representation (2.8 W m-2). An even larger difference (by a factor of 3.5) is found between the estimates of the DRE over the snow-or ice-covered areas. The different treatments of the BB OA evolution are associated also with considerably different contributions of black and brown carbon to the DRE estimates. Overall, our results indicate that model estimates of the DRE of Siberian BB aerosol in the eastern Arctic are strongly sensitive to the assumptions regarding the evolution of OA in Siberian BB plumes and that the SOA formation in these plumes is one of the major factors determining the magnitude of the radiative effects of Siberian BB aerosol in the real atmosphere.

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.