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.

As an important type of light-absorbing aerosol, brown carbon (BrC) has the potential to affect the atmospheric photochemistry and Earth's energy budget. A comprehensive field campaign was carried out along the transport pathway of Asian dust during the spring of 2016, including a desert site (Erenhot), a rural site (Zhangbei), and an urban site (Jinan), in northern China. Optical properties, bulk chemical compositions, and potential sources of water-soluble brown carbon (WS-BrC) were investigated in atmospheric total suspended particulate (TSP) samples. Samples from Zhangbei had higher mass absorption efficiency at 365 nm (MAE(365), 132 +/- 0.34 m(2) g(-1)) than those from Jinan (1.00 +/- 023 m(2) g(-1)) and Erenhot (0.84 +/- 0.30 m(2) g(-1)). Compere to the non-dust samples, elevated water-soluble organic carbon (WSOC) concentrations and MAE 365 values of dust samples from Erenhot are related to the input of high molecular weight organic compounds and biogenic matter from the Gobi Desert, while lower values from Zhangbei and Jinan are attributed to the dilution effect caused by strong northwesterly winds. Based on fluorescence excitation-emission matrix spectra and parallel factor analysis, two humic-like (C1 and C2) and two protein-like (C3 and C4) substances were identified. Together, C1 and C2 accounted for similar to 64% of total fluorescence intensity at the highly polluted urban Jinan site; C3 represented similar to 45% at the rural Zhangbei site where local biomass burning affects; and C4 contributed similar to 24% in the desert region (Erenhot) due to dust-sourced biogenic substances. The relative absorptive forcing of WS-BrC compared to black carbon at 300-400 nm was about 31.3%, 13.9%, and 9.2% during non-dust periods at Erenhot, Zhangbei, and Jinan, respectively, highlighting that WS-BrC may significantly affect the radiative balance of Earth's climate system and should be included in radiative forcing models. (C) 2021 Elsevier B.V. All rights reserved.

According to satellite monitoring data (MODIS/Terra), the spatial distribution of the aerosol optical depth (AOD) at a wavelength of 550 nm for the summer smog of 2007 over the North China Plain (NCP) and adjacent areas has been obtained. Areas over which the AOD is higher due to regional anthropogenic contamination sources near Beijing and Shanghai, as well as the smoke haze forming due to agricultural burning (the southwest part of the NCP), have been revealed. The similarity of optical and microphysical characteristics of aerosol in the smoke haze over the NCP and in the Russian territory has been found: (i) the decisive contribution to the optical characteristics of smoke aerosol is made by the fine mode and (ii) the attenuation spectra in the wavelength region 340-1020 nm are approximated (in logarithmic coordinates) by parabolas or fourth degree polynomials. The monitoring data at the AERONET Beijing site show that the single scattering albedo in the summer smog over the NCP is on average less (0.91) than in the smoke haze in the Russian territory (0.95-0.96). The radiative regimes of the atmosphere are significantly different: in the smog, the aerosol radiative forcing efficiency is lower approximately by 30% at the top of the atmosphere and higher by 30% at the bottom of the atmosphere than in the smoke haze.

Tar balls are frequently found in slightly aged biomass burning plumes. They are spherical in shape, have diameters between similar to 100 and 300 nm, are amorphous and composed mostly of oxygen and carbon. Tar balls are light absorbing and considered to be a component of brown carbon. Tar balls have been typically reported and analyzed as individual spheres: however, in a recent study, we reported the presence of significant fractions of fractal-like aggregates made of several tar balls in fire plumes from different geographical locations. Aggregation affects the optical properties of particles; therefore, we use T-Matrix and Lorenz-Mie simulations to explore the effects of aggregation on the tar balls' optical properties in the 350 - 1150 nm wavelength range. We also evaluate the effects of different refractive indices available from the literature, different monomer numbers, and monomer sizes, as these are key factors determining the aggregates optical properties. Furthermore, we estimate the simple forcing efficiency for low and high surface albedos. Aggregates have a single scattering albedo (SSA) higher than that of individual tar balls (Delta SSA(550) (nm) up to 0.22). The hemispherical upscatter fraction of individual tar balls is more than 100% larger than for tar ball aggregates in many cases. The top of the atmosphere simple forcing efficiency over dark surfaces shows large variabilities with an increase up to similar to 53% for tar ball aggregates compared to individual tar balls. These results demonstrate that aggregation of tar balls can have a significant impact on their optical properties and radiative forcing. (C) 2019 Elsevier Ltd. All rights reserved.

The strategic location of the AERONET site in Ilorin, Nigeria, makes it possible to obtain information on several aerosol types and their radiative effects. The strong reversal of wind direction occasioned by the movement of the ITCZ during the West Africa Monsoon (WAM) plays a major role in the variability of aerosol nature at this site, which is confirmed by aerosol optical depth (AOD) (675 nm) and angstrom ngstrom exponent (AE) (440-870 nm) values with 1st and 99th percentile values of 0.08 and 2.16, and 0.11 and 1.47, respectively. The direct radiative forcing (DRF) and radiative forcing efficiency (RFE) of aerosol, as retrieved from the AERONET sun-photometer measurements, are estimated using radiative transfer calculations for the periods of 2005-2009 and 2011-2015. The DRF and RFE of the dominant aerosol classes-desert dust (DD), biomass burning (BB), urban (UB) and gas flaring (GF)-have been estimated. The median (+/- standard deviation) values of the DRF at the top of the atmosphere (TOA) for the DD, BB, UB and GF aerosol classes are -27.5 +/- 13.2 Wm(-2), -27.1 +/- 8.3 Wm(-2), -11.5 +/- 13.2 Wm(-2) and -9.6 +/- 8.0 Wm(-2), respectively, while those of the RFE are -26.2 +/- 4.1 Wm(-2) delta(-1), -35.2 +/- 4.6 Wm(-2) delta(-1), -31.0 8.4 Wm(-2) delta(-1) and -37.0 +/- 10.3 Wm(-2) delta(-1), respectively. Arguably due to its high SSA and assymetric values, the DD aerosol class shows the largest DRF but the smallest RFE. Its smallest AOD notwithstanding, the GF class can cause greater perturbation of the earth-atmosphere system in the sub-region both directly and indirectly, possibly due to the presence of black carbon and other co-emitted aerosol and the ageing of the GF aerosols. This study presents the first estimate of DRF for aerosols of gas flaring origin and shows that its radiative potential can be similar in magnitude to that of biomass burning and urban aerosol in West Africa.

The focus of present paper is upon aerosol variability in Bucharest metropolitan area and its relationships with aerosol direct effect/forcing (DRE/DRF). The aerosol (particulate matter less than 10 mu m, PM10) mass concentrations were collected at three sampling sites (within a grid-scale of a regional climate model) covering three types of pollution (urban, suburban, and rural) in Bucharest area during 1st of June 2014 to 31st of May 2015. The aerosol optical properties were computed using the Optical Properties of Aerosol and Clouds (OPAC) software package, based on Mie scattering theory. We observed relatively high levels of PM10 with moderate to low seasonal cycle. DRF values indicate a cooling aerosol effect and show annual variations due to the combined effects of variability of aerosol optical properties over Bucharest region and of local geophysical variables. A dedicated to comparison of aerosol DRF and its efficiency in Bucharest area and worldwide is included.

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.

The impact of biomass burning (BB) on aerosol optical properties and radiative budget in the polar region following an intense boreal fire event in North America in July 2015 is explored in this paper. Presented data are obtained from the Navy Aerosol Analysis and Prediction System (NAAPS) reanalysis and the Fu-Liou radiative transfer model. NAAPS provides particle concentrations and aerosol optical depth (AOD) at 1 degrees x 1 degrees spatial and 6 hourly temporal resolution, its AOD and vertical profiles were validated with field measurements for this event. Direct aerosol radiative forcings (ARF) at the surface, the top of the atmosphere (TOA) and within the atmosphere are calculated for clear-sky and all-sky conditions, with the surface albedo and cloud properties constrained by satellite retrievals. The mean ARFs at the surface, the TOA, and within the atmosphere averaged for the north pole region (latitudes north of 75.5N) and the study period (July 5-15, 2015) are -13.1 +/- 2.7, 0.3 +/- 2.1, and 13.4 +/- 2.7 W/m(2) for clear-sky and -7.3 +/- 1.8, 5.0 +/- 2.6, and 12.3 +/- 1.6 W/m(2) for all-sky conditions respectively. Local ARFs can be a several times larger e.g. the clear-sky surface and TOA ARF reach over Alaska 85 and 30 W/m(2) and over Svalbard 41 and 20 W/m(2) respectively. The ARF is found negative at the surface (almost zero over high albedo region though) with the maximum forcing over the BB source region, and weaker forcing under all-sky conditions compared to the clear-sky conditions. Unlike the ARFs at the surface and within the atmosphere, which have consistent forcing signs all over the polar region, the ARF at the TOA changes signs from negative (cooling) over the source region (Alaska) to positive (heating) over bright surfaces (e.g., Greenland) because of strong surface albedo effect. NAAPS simulations also show that the transported BB particle over the Arctic are in the low-to-middle troposphere and above low-level clouds, resulting in little difference in ARFs at the TOA between clear- and all-sky conditions over the regions with high surface albedo. Over dark surfaces, the negative TOA forcing increases with AOD about 50% slower under all-sky conditions compared to clear-sky case. The boreal BB event resulted in large magnitude of ARFs and the high variabilities of the forcings over the polar region has a significant impact on the polar weather conditions and important implications for the polar climate.

Accurate information about aerosol vertical distribution is needed to reduce uncertainties in aerosol radiative forcing and its effect on atmospheric dynamics. The present study deals with synergistic analyses of aerosol vertical distribution and aerosol optical depth (AOD) with meteorological variables using multisatellite and ground-based remote sensors over Kanpur in central Indo-Gangetic Plain (IGP). Micro-Pulse Lidar Network-derived aerosol vertical extinction (sigma) profiles are analyzed to quantify the interannual and daytime variations during monsoon onset period (May-June) for 2009-2011. The mean aerosol profile is broadly categorized into two layers viz., a surface layer (SL) extending up to 1.5km (where sigma decreased exponentially with height) and an elevated aerosol layer (EAL) extending between 1.5 and 5.5km. The increase in total columnar aerosol loading is associated with relatively higher increase in contribution from EAL loading than that from SL. The mean contributions of EALs are about 60%, 51%, and 50% to total columnar AOD during 2009, 2010, and 2011, respectively. We observe distinct parabolic EALs during early morning and late evening but uniformly mixed EALs during midday. The interannual and daytime variations of EALs are mainly influenced by long-range transport and convective capacity of the local emissions, respectively. Radiative flux analysis shows that clear-sky incoming solar radiation at surface is reduced with increase in AOD, which indicates significant cooling at surface. Collocated analysis of atmospheric temperature and aerosol loading reveals that increase in AOD not only resulted in surface dimming but also reduced the temperature (approximate to 2-3 degrees C) of lower troposphere (below 3km altitude). Radiative transfer simulations indicate that the reduction of incoming solar radiation at surface is mainly due to increased absorption by EALs (with increase in total AOD). The observed cooling in lower troposphere in high aerosol loading scenario could be understood as a dynamical feedback of EAL-induced stratification of lower troposphere. Further, the observed radiative effect of EALs increases the stability of the lower troposphere, which could modulate the large-scale atmospheric dynamics during monsoon onset period. These findings encourage follow-up studies on the implication of EALs to the Indian summer monsoon dynamics using numerical models.