China is an important emitter of light-absorbing carbonaceous aerosols (LACs), including black carbon (BC) and brown carbon (BrC). Currently, there are large uncertainties in model-estimated direct radiative forcing (DRF) of LACs, partially due to the poor understanding of the emissions and optical properties of LACs. In this study, we estimated the DRF of LACs over China during the implementation of the Air Pollution Prevention and Control Action Plan (APPCAP) using the global chemical transport model (GEOS-Chem) coupled with the Rapid Radiative Transfer Model of GCMs (RRTMG). We updated the refractive index of BC, includedbiomass burning (BB) sources, biofuel (BF) and coal combustion (CC) sources in the residential sector as BrC emission sources and the optical properties were updated, which were not fully considered in the previous model studies. Our results showed that model could reasonably capture the spatial and temporal variations of LACs in China with the correlation coefficients between model simulated and Aerosol Robotic Network (AERONET) observed daily absorption aerosol optical depth (AAOD) of LACs at 440 nm above 0.63 and the corresponding values of the normalized mean bias within +/- 30%. The simulated annual mean LACs AAOD at 440 nm in China was 0.016 (0.021) in 2017 (2014) and BrC contributed about 20% (21%). The estimated annual mean clear-sky LACs DRF at the top of the atmosphere in China was 1.02 W m(-2) in 2017 and 1.38 W m(-2) in 2014, and the contribution of BrC was about 10% and 11%, respectively, which was dominated by the BF sources (46% in 2017 and 44% in 2014) and the BB sources (38% in 2017 and 43% in 2014), with CC sources being low (16% in 2017 and 13% in 2014). The annual mean AAOD and DRF of LACs in China decreased by 0.005 and 0.36 W m(-2) from 2014 to 2017, which were largely attributed to the reductions of anthropogenic emissions during the implementation of APPCAP. Our results would improve the understanding of the light absorption capacity and climate effects of LACs in China.

Brown carbon (BrC) aerosols have important warming effects on Earth's radiative forcing. However, information on the evolution of the light-absorption properties of BrC aerosols in the Asian outflow region is limited. In this study, we evaluated the light-absorption properties of BrC using in-situ filter measurements and sky radiometer observations of the ground-based remote sensing network SKYradiometer NETwork (SKYNET) made on Fukue Island, western Japan in 2018. The light-absorption coefficient of BrC obtained from filter measurements had a temporal trend similar to that of the ambient concentration of black carbon (BC), indicating that BrC and BC have common combustion sources. The absorption Angstrom exponent in the wavelength range of 340-870 nm derived from the SKYNET observations was 15% higher in spring (1.81 +/- 0.30) than through the whole year (1.53 +/- 0.50), suggesting that the Asian outflow carries light-absorbing aerosols to Fukue Island and the western North Pacific. After eliminating the contributions of BC, the absorption Angstrom exponent of BrC alone obtained from filter observations had a positive Spearman correlation (r(s) = 0.77, p < 0.1) with that derived from SKYNET observations but 33% higher values, indicating that the light-absorption properties of BrC were suc-cessfully captured using the two methods. Using the atmospheric transport model FLEXPART and fire hotspots obtained from the Visible Infrared Imaging Radiometer Suite product, we identified a high-BrC event related to an air mass originating from regions with consistent fossil fuel combustion and sporadic open biomass burning in central East China. The results of the study may help to clarify the dynamics and climatic effects of BrC aerosols in East Asia. (C) 2021 Elsevier B.V. All rights reserved.

Black carbon (BC) exerts important radiative effects over regions with intensive emissions. This study presents in-situ aircraft measurements of BC vertical profiles including mass loading, size distribution and mixing state, spanning a range of pollution levels in both warm and cold seasons over Beijing. The development of planetary boundary layer (PBL) influenced the properties of pollutants at low levels, and regional transport from the southwest elevated the pollution at higher altitudes. Thicker coatings of BC were associated with higher pollution in the PBL, where interactions between BC and other substances intensively took place. Considering the mixing state of BC, the absorption efficiency could be potentially increased by up to 86% and 60% in the PBL and lower free troposphere, respectively. Including a columnintegrated absorption enhancement, the in-situ constrained absorption aerosol optical depth at wavelength 870 nm (AAOD(870)) improved the agreement with AERONET by 28%, but the in-situ measurement remained 19% lower. A radiative transfer model finds a BC heating rate of 0.1-0.3 K/d and 0.5-3.1 K/d for less and more polluted environments respectively, and the BC coating effect could positively introduce a +0.1-4.2 Wm(-2) radiative forcing. The presence of aerosol layer enhanced the positive vertical gradient of heating rate by redistributing the actinic flux. In particular, this gradient was further enhanced by introducing thickly-coated BC at higher level during the regional transport events, which may promote the temperature inversion and further depress the PBL development on polluted days. (C) 2020 Elsevier Ltd. All rights reserved.

Absorption aerosol optical depth (AAOD) measurements made by sun-sky photometers are currently the only constraint available for estimates of the global radiative forcing of black carbon (BC), but their validation studies are limited. In this paper, we report the first attempt to compare AAODs derived from single-particle soot photometer (SP2) and ground-based sun-sky photometer (sky radiometer, SKYNET) measurements. During the Aerosol Radiative Forcing in East Asia (A-FORCE) experiments, BC size distribution and mixing state vertical profiles were measured using an SP2 on board a research aircraft near the Fukue Observatory (32.8 degrees N, 128.7 degrees E) over the East China Sea in spring 2009 and late winter 2013. The aerosol extinction coefficients (b(ext)) and single scattering albedo (SSA) at 500 nm were calculated based on aerosol size distribution and detailed BC mixing state information. The calculated aerosol optical depth (AOD) agreed well with the sky radiometer measurements (26%) when dust loadings were low (lidar-derived nonspherical particle contribution to AOD less than 20%). However, under these low-dust conditions, the AAODs obtained from sky radiometer measurements were only half of the in situ estimates. When dust loadings were high, the sky radiometer measurements showed systematically higher AAODs even when all coarse particles were assumed to be dust for in situ measurements. These results indicate that there are considerable uncertainties in AAOD measurements. Uncertainties in the BC refractive index, optical calculations from in situ data, and sky radiometer retrieval analyses are discussed.