Atmospheric Brown Carbon (BrC) with strong wavelength-dependence light-absorption ability can significantly affect radiative forcing. Highly resolved emission inventories with lower uncertainties are important premise and essential in scientifically evaluating impacts of emissions on air quality, human health and climate change. This study developed a bottom-up inventory of primary BrC from combustion sources in China from 1960 to 2016 with a spatial resolution at 0.1 degrees x 0.1 degrees, based on compiled emission factors and detailed activity data. The primary BrC emission in China was about 593 Gg (500-735 Gg as interquartile range) in 2016, contributing to 7% (5%-8%) of a previously estimated global total BrC emission. Residential fuel combustion was the largest source of primary BrC in China, with the contribution of 67% as the national average but ranging from 25% to 99% among different provincial regions. Significant spatial disparities were also observed in the relative shares of different fuel types. Coal combustion contribution varied from 8% to 99% across different regions. Heilongjiang and North China Plain had high emissions of primary BrC. Generally, on the national scale, spatial distribution of BrC emission density per area was aligned with the population distribution. Primary BrC emission from combustion sources in China have been declined since a peak of similar to 1300 Gg in 1980, but the temporal trends were distinct in different sectors. The high-resolution inventory developed here enables radiative forcing simulations in future atmospheric models so as to promote better understanding of carbonaceous aerosol impacts in the Earth's climate system and to develop strategies achieving co-benefits of human health protection and climate change.

Brown carbon (BrC) has been recognized as an important light-absorbing carbonaceous aerosol, yet understanding of its influence on regional climate and air quality has been lacking, mainly due to the ignorance of regional coupled meteorology-chemistry models. Besides, assumptions about its emissions in previous explorations might cause large uncertainties in estimates. Here, we implemented a BrC module into the WRF-Chem model that considers source-dependent absorption and avoids uncertainties caused by assumptions about emission intensities. To our best knowledge, we made the first effort to consider BrC in a regional coupled model. We then applied the developed model to explore the impacts of BrC absorption on radiative forcing, regional climate, and air quality in East Asia. We found notable increases in aerosol absorption optical depth (AAOD) in areas with high OC concentrations. The most intense forcing of BrC absorption occurs in autumn over Southeast Asia, and values could reach around 4 W m(-2). The intensified atmospheric absorption modified surface energy balance, resulting in subsequent declines in surface temperature, heat flux, boundary layer height, and turbulence exchanging rates. These changes in meteorological variables additionally modified near-surface dispersion and photochemical conditions, leading to changes of PM2.5 and O-3 concentrations. These findings indicate that BrC could exert important influence in specific regions and time periods. A more in-depth understanding could be achieved later with the developed model.

The Black carbon (BC) and Brown carbon (BrC) concentration has been measured over Srinagar (Garhwal) in central Himalayas during October 2020 to September 2021 periods. The average BC mass was 2.59 +/- 1.96 mu g m- 3 and its absorption coefficients were abundant at shorter wavelength. BC seasonal variation exhibited a significant variability, with highest during winter (4.54 +/- 2.64 mu g m- 3) followed by pre-monsoon (2.69 +/- 2.04 mu g m- 3) and post-monsoon (1.93 +/- 0.91 mu g m- 3) while lowest was observed in the monsoon (1.05 +/- 0.54 mu g m- 3). Relatively high contribution of total spectral light absorption coefficient (Abs lambda) was observed (75.94 Mm-1) at 370 nm than longer wavelength (16.86 Mm-1) at 950 nm. The BrC contribution was higher at 370 nm (32.50 Mm-1) to the total babs (lambda), while at higher wavelengths it has extensively decreased (2.54 Mm-1 at 660 nm). Seasonally, the absorption coefficient of BC and BrC was greater in winter (83.99 and 68.37 Mm-1) while lowest in monsoon (19.38 and 9.27 Mm-1), respectively. The babs BrC/babs (t) ratio revealed higher contribution of BrC in winters. The secondary brown carbon (BrCsec) and primary brown carbon (BrCpri) contributed 43.16 % and 56.88 % towards the total BrC Abs (lambda) at 370 nm with higher in winter and lowest in monsoon, respectively. BrCsec and BrCprim has shown higher contribution in evening (18.00-20.00 h) and in morning (09.00-11.00 h) hours. The average radiative forcing (RF) of BC was 36.11 +/- 6.99 Wm-2, 2.19 +/- 1.22 Wm-2 and -33.92 +/- 5.96 Wm-2 at the atmosphere (ATM), Top of the Atmosphere (TOA), and at the Surface (SUR), respectively.

Light-absorbing carbonaceous aerosols that dominate atmospheric aerosol warming over India remain poorly characterized. Here, we delve into UV-visible-IR spectral aerosol absorption properties at nine PAN-India COALESCE network sites (Venkataraman et al., 2020, ). Absorption properties were estimated from aerosol-laden polytetrafluoroethylene filters using a well-constrained technique incorporating filter-to-particle correction factors. The measurements revealed spatiotemporal heterogeneity in spectral intrinsic and extrinsic absorption properties. Absorption analysis at near-UV wavelengths from carbonaceous aerosols at these regional sites revealed large near-ultraviolet brown carbon absorption contributions from 21% to 68%-emphasizing the need to include these particles in climate models. Further, satellite-retrieved column-integrated absorption was dominated by surface absorption, which opens possibilities of using satellite measurements to model surface-layer optical properties (limited to specific sites) at a higher spatial resolution. Both the satellite-modeled and direct in-situ absorption measurements can aid in validating and constraining climate modeling efforts that suffer from absorption underestimations and high uncertainties in radiative forcing estimates. Particulate pollution in the atmosphere scatter and absorb incoming solar energy, thus cooling or warming Earth's atmosphere. In developing countries and especially in India, one of the most polluted regions of the world, the extent to which particles can absorb solar energy and warm the atmosphere is not well understood. Here, for the first time, we measure particle absorption simultaneously at nine ground sites across India, in diverse geographical regions with different levels and types of particulate pollution. We find that organic carbon particles exert large absorption at near-ultraviolet wavelengths, which contain significant solar energy. These light absorbing organic carbon particles, called brown carbon, are emitted in large quantities from biomass burning (e.g., burning crop residue and cooking on wood-fired stoves). Comparing ground measurements of absorption with satellite-retrieved measurements that are representative of the entire atmospheric column, we find that near-surface atmospheric particles can exert significant warming. This study highlights the need to improve climate model simulations of particulate pollution's impact on the climate by incorporating spatiotemporal surface-level absorption measurements, including absorption by brown carbon particles. Measurements at nine regional PAN-India sites reveal several regions with large aerosol absorption strength Brown carbon contributes significantly (21%-68%) to near-ultraviolet absorption, indicating its importance in shortwave light absorption Strong correlations observed between satellite data and surface absorption indicate future potential in modeling surface absorption

To elucidate the variations in mass concentrations of organic carbon (OC) and black carbon (BC) in PM2s and their light absorption characteristics in Lanzhou, we conducted one-year online measurements by using a newly developed total carbon analyzer (TCA08) coupled with an aethalometer (AE33) from July 2018 to July 2019. The mean OC and BC concen-trations were 6.4 +/- 4.4 and 2.0 +/- 1.3 pg/m3, respectively. Clear seasonal variations were observed for both components, with winter having the highest concentrations, followed by autumn, spring, and summer. The diurnal variations of OC and BC concentrations were sim-ilar throughout the year, with daily two peaks occurring in the morning and evening, respec-tively. A relatively low OC/BC ratio (3.3 +/- 1.2, n = 345) were observed, indicating that fossil fuel combustion was the primary source of the carbonaceous components. This is further substantiated by relatively low biomass burning contribution (fbiomass: 27.1% +/- 11.3%) to BC using aethalometer based measurement though f biomass value which increased significantly in winter (41.6% +/- 5.7%). We estimated a considerable brown carbon (BrC) contribution to the total absorption coefficient (babs) at 370 nm (yearly average of 30.8% +/- 11.1%), with a win-ter maximum of 44.2% +/- 4.1% and a summer minimum of 19.2% +/- 4.2%. Calculation of the wavelength dependence of total babs revealed an annual mean AAE370-520 value of 4.2 +/- 0.5, with slightly higher values in spring and winter. The mass absorption cross- of BrC also exhibited higher values in winter, with an annual mean of 5.4 +/- 1.9 m2middotg-1 , reflecting the impact of emissions from increased biomass burning on BrC concentrations.(c) 2022 The Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences. Published by Elsevier B.V.

As an important component of organic carbon (OC), brown carbon (BrC) plays a significant role in radiative forcing in the atmosphere. Water-insoluble OC (WIOC) generally has higher light absorption ability than water-soluble OC (WSOC). The mass absorption cross- (MAC) of WIOC is normally investigated by dissolving OC in methanol. However, all the current methods have shortcomings due to neglecting the methanol insoluble particulate carbon that is detached from the filter and suspended in methanol extracts, which results in MAC uncertainties of the methanol-soluble BrC and its climate warming estimation. In this study, by investigating typical biomass combustion sourced aerosols from the Tibetan Plateau and ambient aerosols from rural and urban areas in China, we evaluated the light absorption of extractable OC fraction for the existing methods. Moreover, a new method was developed to overcome the methanol insoluble particulate carbon detachment problem to achieve more reliable MAC values. We found that OC can be dissolved in methanol in a short time (e.g., 1 h) and ultrasonic treatment and long-term soaking do not significantly increase the extractable OC fraction. Additionally, we proved that methanol insoluble particulate carbon detachment in methanol does exist in previous methods, causing overestimation of the BrC mass extracted by methanol and thus the underestimation of MAC values. We therefore recommend the newly developed extraction method in this study to be utilized in future related studies to quantitatively obtain the light absorption property of methanol-soluble BrC. (C) 2020 Elsevier Ltd. All rights reserved.

Aerosol chemical components such as black carbon (BC) and brown carbon (BrC) regulate aerosol optical properties, which in turn drive the atmospheric radiative forcing estimations due to aerosols. In this study, we used the long-term measurements from AERONET (Aerosol Robotic Network) to better understand the aerosol types and composition with respect to their seasonal and spatial variabilities in peninsular Southeast Asia (PSEA, here defined as Vietnam, Cambodia, Thailand, Laos, and Myanmar). Two methods (i.e., aerosol type cluster and aerosol component retrieval) were applied to determine the aerosol type and chemical composition during the biomass-burning (BB) season. AERONET sites in northern PSEA showed a higher AOD (aerosol optical depth) compared to that of southern PSEA. Differences in land use pattern, geographic location, and weather regime caused much of the aerosol variability over PSEA. Lower single-scattering albedo (SSA) and higher fine-mode fraction (FMF) values were observed in February and March, suggesting the predominance of BB type aerosols with finer and stronger absorbing particles during the dry season. However, we also found that the peak BB month (i.e., March) in northern PSEA may not coincide with the lowest SSA once dust particles have mixed with the other aerosols. Furthermore, we investigated two severe BB events in March of 2014 and 2015, revealing a significant BrC fraction during BB event days. On high AOD days, although the BC fraction was high, the BrC fraction remained low due to lack of aerosol aging. This study highlights the dominance of carbonaceous aerosols in the PSEA atmosphere during the BB season, while also revealing that transported dust particles and BrC aerosol aging may introduce uncertainties into the aerosol radiative forcing calculation.

South and Southeast Asia (SSA) emitted black carbon (BC) exerts potential effects on glacier and snow melting and regional climate change in the Tibetan Plateau. In this study, online BC measurements were conducted for 1 year at a remote village located at the terminus of the Mingyong Glacier below the Meili Snow Mountains. The Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) was used to investigate the contribution and potential effect of SSA -emitted BC. In addition, variations in the light absorption characteristics of BC and brown carbon (BrC) were examined. The results indicated that the annual mean concentration of BC was 415 +/- 372 ngm(-3) , with the highest concentration observed in April (monthly mean: 930 +/- 484 ngm(-3) ). BC exhibited a similar diurnal variation throughout the year, with two peaks observed in the morning (from 8:00 to 9:00 AM) and in the afternoon (from 4:00 to 5:00 PM), with even lower values at nighttime. At a short wavelength of 370 nm, the absorption coefficient ( b abs ) reached its maximum value, and the majority of b abs values were < 20 Mm(-1) , indicating that the atmosphere was not overloaded with BC. At the same wavelength, BrC substantially contributed to b abs , with an annual mean of 25.2 % +/- 12.8 %. SSA was the largest contributor of BC (annual mean: 51.1 %) in the study area, particularly in spring (65.6 %). However, its contributions reached 20.2 % in summer, indicating non -negligible emissions from activities in other regions. In the atmosphere, the SSA BC -induced radiative forcing (RF) over the study region was positive. While at the near surface, the RF exhibited a significant seasonal variation, with the larger RF values occurring in winter and spring. Overall, our findings highlight the importance of controlling BC emissions from SSA to protect the Tibetan Plateau against pollution -related glacier and snow cover melting.

The optical properties of secondary brown carbon (BrC) aerosols are poorly understood, hampering quantitative assessments of their impact. We propose a new method for estimating secondary source of BrC using excitation-emission matrix (EEM) fluorescence spectroscopy, combined with parallel factor analysis (PARAFAC) and partial least squares regression (PLSR). Experiments were conducted on a collection of PM2.5 samples from urban areas in five Chinese cities during winter and summer. The humic-like component with long-emission wavelengths (L-HULIS) was identified as a secondary source tracer of BrC. This was confirmed by correlating PARAFAC components with secondary organic aerosol tracers and molecular oxidation indices obtained from Fourier transform ion cyclotron resonance mass spectrometry analysis. Using L-HULIS as a secondary tracer of BrC, it was determined that the contribution of secondary sources to water-soluble BrC (WS-BrC) in source emission samples is significantly smaller than in PM2.5 from five Chinese cities, supporting our method. In the five cities, secondary source derived via L-HULIS contributes a dominant potion (80% +/- 3.5%) of WS-BrC at 365 nm during the summer, which is approximately twice as high as during the winter (45% +/- 4.9%). Radiocarbon isotope (14C) analysis provides additional constraints to the sources of L-HULIS-derived secondary WS-BrC in urban PM2.5, suggesting that aged biomass burning is the dominant contributor to secondary WS-BrC in winter, and biogenic emission is dominant during summer. This study is the first report on identification of secondary sources of BrC using the fluorescence technique. It demonstrates the potential of this method in characterizing non-fossil source secondary BrC in the atmosphere. Brown carbon (BrC) originates from primary combustion emissions and secondary formation, with large source-dependent uncertainties of radiative forcing. Direct measurements to separate the primary and secondary BrC are challenging due to the chemical complexity. Recent online studies have shown that excitation-emission matrix fluorescence spectroscopy coupled with parallel factor (PARAFAC) analysis identified some fluorescent components that may be linked to secondary sources. However, there is a knowledge gap on whether PARAFAC components correlate closely with atmospheric secondary chemical components, particularly biogenic and anthropogenic secondary organic aerosol, as their precursors can also form secondary BrC chromophores. We established the correlations between PARAFAC components and secondary organic aerosol tracers and compound oxidations to identify the long-emission-wavelength humic-like component as a secondary source tracer of BrC. Then, we estimated non-fossil source secondary BrC in urban aerosols during the winter and summer. Our studies provide references for quantifying secondary sources of BrC in the atmosphere. A fluorescence-based method was developed to investigate secondary sources of water-soluble brown carbon in five cities in China The contribution of secondary sources to water-soluble brown carbon in the summer is approximately twice as high as during the winter This secondary water-soluble brown carbon was more associated with aging biomass burning in winter and biogenic emissions in summer

The NO3 center dot-driven nighttime aging of brown carbon (BrC) is known to greatly impact its atmospheric radiative forcing. However, the impact of oxidation by NO3 center dot on the optical properties of BrC in atmospheric waters as well as the associated reaction mechanism remain unclear. In this work, we found that the optical variation of BrC proxies under environmentally relevant NO3 center dot exposure depends strongly on their sources, with enhanced light absorptivity for biomass-burning BrC but bleaching for urban aerosols and humic substances. High-resolution mass spectrometry using FT-ICR MS shows that oxidation by NO3 center dot leads to the formation of light-absorbing species (e.g., nitrated organics) for biomass-burning BrC while destroying electron donors (e.g., phenols) within charge transfer complexes in urban aerosols and humic substances, as evidenced by transient absorption spectroscopy and NaBH4 reduction experiments as well. Moreover, we found that the measured rate constants between NO3 center dot with real BrCs (k = (1.8 +/- 0.6) x 10(7) M(C)(-1)s(-1), expressed as moles of carbon) are much higher than those of individual model organic carbon (OC), suggesting the reaction with OCs may be a previously ill-quantified important sink of NO3 center dot in atmospheric waters. This work provides insights into the kinetics and molecular transformation of BrC during the oxidation by NO3 center dot, facilitating further evaluation of BrC's climatic effects and atmospheric NO3 center dot levels.