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.

Carbonaceous aerosols were collected in the valley city of Baoji city in Northern China in August 2022. The light absorption characteristics and influencing factors of black carbon (BC) and brown carbon (BrC) were analyzed, and their radiative forcing was estimated. The results showed that the light absorption of secondary brown carbon [AbsBrC,sec (370)] was 7.5 +/- 2.4 Mm(-1), which was 2.5 times that of primary brown carbon [AbsBrC,pri (370), 3.0 +/- 1.2 Mm(-1)]. During the study period, the absorption Angstrom exponent (AAE) of aerosol was 1.6, indicating that there was obvious secondary aerosol formation or carbonaceous aerosol aging in the valley city of Baoji. Except for secondary BrC (BrCsec), the light absorption coefficient (Abs) and mass absorption efficiency (MAE) of BC and primary BrC (BrCpri) during the persistent high temperature period (PHT) were higher than those during the normal temperature period (NT) and the precipitation period (PP), which indicated that the light absorption capacity of black carbon and primary brown carbon increased, while the light absorption capacity of secondary brown carbon decreased under persistent high temperature period. Secondary aerosols sulfide (SO42-), nitrate (NO3-) and secondary organic carbon (SOC) are important factors for promoting the light absorption enhancemen of BC and BrCpri and photobleaching of BrCsec during persistent high temperature period. The Principal Component Analysis-Multiple Linear Regression (PCA-MLR) model showed that traffic emissions was the most important source of pollution in Baoji City. Based on this, the secondary source accelerates the aging of BC and BrC, causing changes in light absorption. During PHT, the radiative forcing of BC and BrCpri were enhanced, while the radiative forcing of BrCsec was weakened, but the positive radiative forcing generated by them may aggravate the high-temperature disaster.

PM2.5 samples (n = 34) were collected from January to April 2017 over Shillong (25.7 degrees N, 91.9 degrees E; 1064 m amsl), a high-altitude site situated in the northeastern Himalaya. The main aim was to understand the sources, characteristics, and optical properties of local vs long-range transported carbonaceous aerosols (CA) using chemical species and dual carbon isotopes (13C and 14C). Percentage biomass burning (BB)/biogenic fraction (fbio, calculated from 14C) varied from 67 to 92 % (78 +/- 7) and correlated well with primary BB tracers like f60, and K+, suggesting BB as a considerable source. Rain events are shown to reduce the fbio fraction, indicating majority of BB-derived CA are transported. Further, delta 13C (-26.6 +/- 0.4) variability was very low over Shillong, suggesting it's limitations in source apportionment over the study region, if used alone. Average ratio of absorption coefficient of methanol-soluble BrC (BrCMS) to water-soluble BrC (BrCWS) at 365 nm was 1.8, indicating a significant part of BrC was water-insoluble. A good positive correlation between fbio and mass absorption efficiency of BrCWS and BrCMS at 365 nm with the higher slope for BrCMS suggests BB derived water-insoluble BrC was more absorbing. Relative radiative forcing (RRF, 300 to 2500 nm) of BrCWS and BrCMS with respect to EC were 11 +/- 5 % and 23 +/- 16 %, respectively. Further, the RRF of BrCMS was up to 60 %, and that of BrCWS was up to 22 % with respect to EC for the samples with fbio >= 0.85 (i.e., dominated by BB), reflecting the importance of BB in BrC RRF estimation.

We report measurements of the optical properties of methanol-soluble organic carbon (MSOC) and water-soluble organic carbon (WSOC) in the metropolitan city of Mumbai (19.01(degrees) N, 72.92(degrees) E), India. The MSOC and WSOC extracts were analysed using UV-visible spectroscopy. The study covered a period of nine months from September 2017 to May 2018. On average, MSOC constituted 30% and WSOC constituted 24% of the PM2.5 mass for the sampling period with peak concentration observed in the winter season. The absorption coefficients of MSOC were on average 1.57 times higher than WSOC for the sampling period. The absorption coefficients of MSOC and WSOC were correlated with the brown carbon absorption coefficients. Mass absorption cross- (MAC) was calculated by normalizing the absorption coefficients with its concentration, and the absorption angstrom exponent (AAE) was calculated by exponential fitting of the absorption coefficients. The MAC values for WSOC were estimated to be 1.03 +/- 0.39 m(2) g(-1), while for MSOC, it was 1.41 +/- 0.76 m(2) g(-1). The relative radiative forcing compared to black carbon was estimated at 10.1 +/- 5.2% and 6.3 +/- 3.8% for MSOC and WSOC, respectively.

The Tibetan Plateau, referred as the last pure land on the earth, is frequently exposure to heavy air pollution during springtime. Here, we find South Asia biomass burning is crucial to cause the heavy springtime air pollution over the Tibetan Plateau, which explain the most (more than 60%) of aerosol components in the region, although its contribution to gaseous pollutants is not significant. South Asian biomass burning mainly affects primary PM2.5 components black carbon (65.3%) and organic carbon (79.5%) over the Tibetan Plateau, but has little influence (less than 5%) on second aerosol components (sulfate, nitrate, and ammonium). The transboundary transmissions of aerosols were regulated by a combination of large-scale westerly winds and regional mountain-valley winds in springtime. In addition to worsen air quality, aerosols from South Asian biomass burning lead to surface temperature decrease of 0.06 degrees C, and precipitation reduction of 3.9 mm over the Tibetan Plateau during springtime. These climate changes will threat the fragile ecosystem over the Tibetan Plateau, such as plant growth and flowering during springtime. Overall, our findings demonstrate a necessary and urgency to reduce biomass burning emissions over South Asia to protect the Tibetan Plateau environment.

With Tibetan Plateau higher than 4 km to the west, the location of Sichuan Basin is unique all around the world and provides a good platform to study air pollution in the urban agglomerations over the complex terrain. To fill in the blanks on vertical distributions of PM1 (the particles smaller than 1 mu m) and carbonaceous aerosols within the basin, by means of high topographic relief, PM1 were off-line sampled during 20 January to 2 February 2018 at eight sites with increasing altitudes from the basin to southeastern margins of the Tibetan Plateau. The regional potential sources for each site were revealed by Hybrid-Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model and concentration-weighted trajectory (CWT) method. The lowest carbonaceous aerosol levels occurred at Lixian, while the highest OC (organic carbon) (EC, elemental carbon) was at Hongyuan (the altitude of 3500 m) (Ande, a rural site) due to more primary emissions. The pollutants inside the basin can be transported the altitudes from 2 km to 3 km by vertical dispersion, but they cannot be dispersed to higher altitudes. The vertical stratification of the pollutants was obvious and easily formed high-low-high pattern from Sichuan Basin to southeastern Tibetan Plateau, especially during highly polluted episodes. The regional potential sources significantly varied as the increased altitudes. Regional pollution was significant inside the basin. The sources at the altitudes from 2 km to 3 km originated from southeastern margins of the Plateau and surrounding cities, while those at higher altitudes were transported from southeastern margins of the Plateau. The impact of basic meteorological variables (temperature, wind speed and vapor pressure) on carbonaceous aerosols was opposite between the basin and Plateau sites. This study was essential to understanding formation mechanisms of severe pollution episodes and thus to making control measures for the urban agglomerations inside the mountainous terrain.

Simultaneous observations (2014-2017) of organic carbon (OC) and elemental carbon (EC) are made over a high-altitude site (Nainital, 29.4 degrees N, 79.5 degrees E, 1958 m a.m.s.l) in the central Himalayas, and the role of long-range transport, meteorology and biomass burning is studied. There are only a few online and simultaneous observations of OC and EC over South Asia and none in the high-altitude Himalayan region. This work presents the first diurnal variations with a unimodal pattern in both OC and EC at the Himalayan site. Such a diurnal pattern is in contrast with the bimodal pattern observed at any continental polluted site. Clear seasonal variations in OC and EC were seen with a primary maximum during spring and a secondary maximum in autumn/winter. OC and EC concentrations are observed to be as high as 65.8 mu g/m(3) and 12 mu g/m(3), in May, respectively. Concentration weighted trajectory (CWT)-assisted analysis shows that the biomass burning in northern India is one of the major sources for the springtime maximum even at this high-altitude site. The coinciding rise in OC/EC ratio from 4.6 to 7.9, along with fire events, further convinces that the enhancement in the concentrations is due to the biomass burning at distant regions and long-range transport of air masses influencing this high-altitude site. A poor covariation between OC-EC and the boundary-layer height during autumn and winter suggests that secondary maxima in OC and EC are most likely due to local sources, e.g. household burning for heating during this cold period when the temperature drops sharply after October and remains low until February. The higher temporal resolution of online measurements reveals that swiftly varying meteorological parameters change the OC-EC concentrations at diurnal scales. Back-air trajectory-assisted analysis of residence time and its relationship with OC and EC confirms the increase in their concentration in slow-moving air masses. The observed diurnal variations of EC are utilized to estimate the radiative forcing and shown that the atmospheric radiative forcing during the afternoon is about 70% higher than the forenoon one. It is envisaged that this dataset with diurnal observations of OC and EC would be an important input for studying the radiation budget and source apportionment over this high-altitude region.

The north-western Indo-Gangetic Plain (IGP) experiences massive crop-residue burning (viz. paddy and wheat) on an annual and seasonal basis. The long-range transport of the particulates emitted from paddyand wheat residue burning (expressed as PRB and WRB, respectively) degrades the air quality, perturb the radiative budget, and alter the atmospheric chemistry of downwind IGP locations. Therefore, chemical, absorption and radiative characteristics of carbonaceous aerosols (total carbon; TC) were explored in this study. The fraction of TC in ambient PM2.5 (particulates with aerodynamic diameter <= 2.5 mu m) was similar to 45% during PRB and similar to 24% during WRB. However, biomass burning emissions were the predominant source of TC during both PRB and WRB. The brown carbon (BrC) aerosols at Beas were similar to 2-3 times more abundant during PRB than in WRB. However, the absorption properties such as mass absorption efficiency and imaginary component of the refractive index for BrC at 405 nm (expressed as MAE(BrC-405), k(BrC-405), respectively) and radiative characteristics such as light absorption capacity were similar during both PRB and WRB. The similarity between these absorption and radiative characteristics indicate that BrC aerosols emitted during the burning of different biomass may depend only on their combustion condition. Further, the increased biomass burning emissions were linked with enhancement in the light absorption capacity of BrC during PRB. A similar light absorption capacity was observed (similar to 30 W/g) for water-soluble BrC (WS-BrC) and total BrC during PRB. Moreover, the % contribution of BrC and EC to their total direct radiative forcing (DRFTC) during PRB and WRB (similar to 40% and similar to 60% for BrC and EC, respectively) were also similar. The WS-BrC constitutes only similar to 15% of DRFTC during PRB. This difference signifies that non-WS-BrC aerosols were the predominant light-absorbing species during PRB (compared to WS-BrC), which needs to be factored into global climate models to mitigate uncertainties.

The lack of light-absorbing aerosols vertical distributions data largely limited to revealing the formation mechanism of severe haze pollution in Chinese cities. Based on the synchronous measurements of size-resolved carbonaceous aerosols and meteorological data at near surface level and hilltop (about 620 m above the valley) in Lanzhou of northwest China, this study compared organic and elemental carbon (OC, EC) size distributions at the two altitudes and revealed the key influencing factors in a typical urban valley, China. The winter OC size distributions were typically bimodal with two comparable peaks in the accumulation and coarse modes, while those in summer were unimodal with the highest value in the size bin of 4.7-5.8 mu m. The size-resolved OC and EC at near the surface were significantly higher than those at the hilltop. The difference (concentrations and size distributions) of OC and EC between the surface and hilltop in summer was much smaller than that in winter due to stronger vertical mixing and larger summer SOC contributions at the hilltop. The winds paralleling with running urban valley were conducive to dispersing the air pollutants from near the surface to the upper air. The roles of horizontal and vertical dispersions to carbonaceous aerosols were comparable at near the surface, while horizontal dispersion was more important at the hilltop. Furthermore, the vertical dispersion was a main factor controlling size-resolved carbonaceous aerosols under highly polluted conditions in a typical urban valley. This study will provide the basis for regulation of severe haze pollution over complex terrain.

The absorption characteristics and source processes of aerosols are investigated at two nearby distinct altitude sites: Nainital, located over the central Himalayas (similar to 1958m amsl) and Pantnagar, in the adjacent foothill region (similar to 231m amsl) in the Indo-Gangetic Plain region (IGP); based on in-situ measurements and model (GEOS-Chem) simulations. The study reveals the significant influence of biomass burning sources over both the locations during spring, indicating the efficiency of the vertical transport of biomass burning aerosols during the peak of the fire activity period over the northern Indian region. On the other hand, the dominance of fossil fuel emission sources is seen during most part of the year at the mountain site, while biomass/biofuel sources are prevalent at the foothill site. Simulations of different aerosol components in the GEOS-Chem model have revealed that dust aerosols, in addition to carbonaceous aerosols from fossil fuel and biomass burning sources, significantly influence aerosol burden over this broad region covering both high-altitude site Nainital and adjacent foothill site Pantnagar in IGP. Examination of dominant aerosol types and their contribution to the columnar abundance of aerosols is performed. During spring, the contribution of dust aerosols is as high as 22%, even though inorganic aerosols (42%), organic carbon (29%) play a dominant role in modulating aerosol absorption characteristics in the column over this region. This study highlights the importance of absorbing aerosol, their types and quantification for better estimates of radiative forcing of aerosols over this region. This might also provide valuable information for the regional impact assessment of aerosols over the Himalayan region.