This study reports day-night and seasonal variations of aqueous brown carbon (BrCaq) and constituent humic-like substances (HULIS) (neutral and acidic HULIS: HULIS-n and HULIS-a) from the eastern Indo-Gangetic Plain (IGP) of India during 2019-2020. This is followed by the application of the receptor model positive matrix factorization (PMF) for optical source apportionment of BrCaq and the use of stable isotopic ratios (813C and 815N) to understand atmospheric processing. Nighttime BrCaq absorption and mass absorption efficiencies (MAE) were enhanced by 40-150 % and 50-190 %, respectively, compared to the daytime across seasons, possibly as a combined effect from daytime photobleaching, dark-phase secondary formation, and increased nighttime emissions. MAE250 nm/MAE365 nm (i.e., E2/E3) ratios and Angstrom Exponents revealed that BrCaq and HULIS-n were relatively more aromatic and conjugated during the biomass burning-dominated periods while BrCaq and HULIS-a were comprised mostly of nonconjugated aliphatic structures from secondary processes during the photochemistry-dominated summer. The relative radiative forcing of BrCaq with respect to elemental carbon (EC) was 10-12 % in the post-monsoon and winter in the 300-400 nm range. Optical source apportionment using PMF revealed that BrCaq absorption at 300, 365 and 420 nm wavelengths in the eastern IGP is mostly from biomass burning (60-75 %), followed by combined marine and fossil fuel-derived sources (24-31 %), and secondary processes (up to 10 %). Source-specific MAEs at 365 nm were estimated to be the highest for the combined marine and fossil fuel source (1.34 m2 g-1) followed by biomass burning (0.78 m2 g-1) and secondary processing (0.13 m2 g-1). Finally, 813C and 815N isotopic analysis confirmed the importance of summertime photochemistry and wintertime NO3--dominated chemistry in constraining BrC characteristics. Overall, the quantitative apportionment of BrCaq sources and processing reported here can be expected to lead to targeted source-specific measurements and a better understanding of BrC climate forcing in the future.

Biomass burning is a major source of Brown Carbon (BrC), strongly contributing to radiative forcing. In urban areas of the climate-sensitive Southeastern European region, where strong emissions from residential wood burning (RWB) are reported, radiative impacts of carbonaceous aerosols remain largely unknown. This study examines the absorption properties of water-and methanol-soluble organic carbon (WSOC, MeS_OC) in a city (Ioannina, Greece) heavily im-pacted by RWB. Measurements were performed during winter (December 2019 - February 2020) and summer (July - August 2019) periods, characterized by RWB and photochemical processing of organic aerosol (OA), respectively. PM2.5 filter extracts were analyzed spectrophotometrically for water-and methanol-soluble BrC (WS_BrC, MeS_BrC) absorption. WSOC concentrations were quantified using TOC analysis, while those of MeS_OC were determined using a newly developed direct quantification protocol, applied for the first time to an extended series of ambient sam-ples. The direct method led to a mean MeS_OC/OC of 0.68 and a more accurate subsequent estimation of absorption efficiencies. The mean winter WS_BrC and MeS_BrC absorptions at 365 nm were 13.9 Mm-1 and 21.9 Mm-1, respec-tively, suggesting an important fraction of water-insoluble OA. Mean winter WS_BrC and MeS_BrC absorptions were over 10 times those observed in summer. MeS_OC was more absorptive than WSOC in winter (mean mass absorption efficiencies - MAE365: 1.81 vs 1.15 m2 gC-1) and especially in summer (MAE: 1.12 vs 0.27 m2 gC-1) due to photo -dissociation and volatilization of BrC chromophores. The winter radiative forcing (RF) of WS_BrC and MeS_BrC rela-tive to elemental carbon (EC) was estimated at 8.7 % and 16.7 %, respectively, in the 300-2500 nm band. However, those values increased to 48.5 % and 60.2 % at 300-400 nm, indicating that, under intense RWB, BrC forcing becomes comparable to that of soot. The results highlight the consideration of urban BrC emissions in radiative transfer models, as a considerable climate forcing factor.

in the atmosphere. Recently, the warming effect of light-absorbing OC has been emphasized. Water-soluble organic carbon (WSOC) is commonly used asa surrogate to investigate the light absorption of OC. Thus far, filters with 0.45 pm (PS1) and 0.20 pm pore sizes (PS2) are both used to investigate the light absorption of WSOC, which may cause large divergent results. In this study, we found that the light absorption ability of WSOC treated with PS1 was higher than that of PS2 due to the extinction of suspended particles (e.g., black carbon) with particle size between 0.20 pm and 0.45 pm, although the concentrations of WSOC treated with PS1 and PS2 were very close. This phenomenon was more remarkable at visible wavelengths, resulting in an overestimation of the warming effect of WSOC by 9%- 22% for aerosol samples treated by PS1, with the highest values occurring in samples heavily influenced by fossil fuel burning emissions. An overestimation of WSOC light absorption treated by PS1 occurred in the investigated ambient aerosol samples from three sites, so it may be a general phenomenon that also exists in other regions of the world. Therefore, to achieve the actual solar radiative forcing of OC in the atmosphere, it is recommended to use PS2 in the future, and reported data of WSOC treated by PS1 should be re-evaluated.

in the atmosphere. Recently, the warming effect of light-absorbing OC has been emphasized. Water-soluble organic carbon (WSOC) is commonly used asa surrogate to investigate the light absorption of OC. Thus far, filters with 0.45 pm (PS1) and 0.20 pm pore sizes (PS2) are both used to investigate the light absorption of WSOC, which may cause large divergent results. In this study, we found that the light absorption ability of WSOC treated with PS1 was higher than that of PS2 due to the extinction of suspended particles (e.g., black carbon) with particle size between 0.20 pm and 0.45 pm, although the concentrations of WSOC treated with PS1 and PS2 were very close. This phenomenon was more remarkable at visible wavelengths, resulting in an overestimation of the warming effect of WSOC by 9%- 22% for aerosol samples treated by PS1, with the highest values occurring in samples heavily influenced by fossil fuel burning emissions. An overestimation of WSOC light absorption treated by PS1 occurred in the investigated ambient aerosol samples from three sites, so it may be a general phenomenon that also exists in other regions of the world. Therefore, to achieve the actual solar radiative forcing of OC in the atmosphere, it is recommended to use PS2 in the future, and reported data of WSOC treated by PS1 should be re-evaluated.

Water-soluble organic carbon (WSOC) widely stored in glaciers from local and distant sources, and then released it to downstream environments under a warming climate. Climatic driven changes to glacial run-off are larger and represent an important flux of organic carbon. However, very few WSOC data are currently available to fully characterize WSOC variation in the temperate glacierized regions of the Tibetan Plateau (TP). This study first systematically evaluated the concentration characteristics and light absorbing property of WSOC, and insoluble particulate carbon (IPC) in snow and ice of a typical temperate glacier on Mt. Yulong. Average concentrations of WSOC were 0.610.21mg L-1 in Baishui glacier on Mt. Yulong. WSOC concentrations in surface aged snow were dramatically decreased with the time extension during the entire monsoon season due to extensive glacial melting and scavenging effects by meltwater.The MAC values of WSOC calculated at 365nm was 6.31 +/- 0.34 m(2) g(-1) on Mt. Yulong, and there exists distinct spectral dependence of MAC(wsoc) within the wavelength range (260-700nm). The low AAE(330-400) values suggest the light absorption of WSOC is more spectrally neutral. The flux of WSOC in Baishui glacier was 0.99 gC m(-2)yr(-1), while the IPC flux was 4.77 gC m(-2)yr(-1). Total WSOC storage in the Baishui glacier was estimated to be 1.5 tone C and total IPC storage was 7.25 tone C (1 tone =10(6)g). Moreover, glacial melting was reinforced by the soluble and insoluble light absorbing impurities (ILAIs) in glaciers, Baishui glacier can be considered as a fraction of carbon source under the scenario of a warming climate, more importantly, WSOC in snow and ice needs to be taken into account in calculating the radiative forcing of ILAIs and accelerating glacial melting.

Brown carbon (i.e., light-absorbing organic carbon, or BrC) exerts important effects on the environment and on climate in particular. Based on spectrophotometric absorption measurements on extracts of bulk aerosol samples, this study investigated the characteristics of BrC during winter in Beijing, China. Organic compounds extractable by methanol contributed approximately 85% to the organic carbon (OC) mass. Light absorption by the methanol extracts exhibited a strong wavelength dependence, with an average absorption Angstrom exponent of 7.10 (fitted between 310 and 450 nm). Normalizing the absorption coefficient (babs) measured at 365 nm to the extractable OC mass yielded an average mass absorption efficiency (MAE) of 1.45 m(2)/g for the methanol extracts. This study suggests that light absorption by BrC could be comparable with black carbon in the spectral range of near-ultraviolet light. Our results also indicate that BrC absorption and thus BrC radiative forcing could be largely underestimated when using water-soluble organic carbon (WSOC) as a surrogate for BrC. Compared to previous work relying only on WSOC, this study provides a more comprehensive understanding of BrC aerosol based on methanol extraction. (C) 2015 Elsevier Ltd. All rights reserved.

The mass absorption efficiency (MAE) of light absorbing water-soluble organics, representing a significant fraction of brown carbon (BrC), has been studied in fine mode aerosols (PM2.5) from a source region (Patiala: 30.2 degrees N, 76.3 degrees E) of biomass burning emissions (BBEs) in the Indo-Gangetic Plain (IGP). The mass absorption coefficient of BrC at 365 nm (b(abs-365)), assessed from absorption spectra of aqueous extracts, exhibits significant linear relationship with water-soluble organic carbon (WSOC) for day (R-2 = 0.37) and night time (R-2 = 0.77) samples; and slope of regression lines provides a measure of MAE of BrC (daytime: similar to 0.75 m(2) g(-1) and night time: 1.13 m(2) g(-1)). A close similarity in the temporal variability of b(abs-365) (for BrC) and K+ in all samples suggests their common source from BBEs. The b(abs-365) of BrC follows a power law (b(abs-lambda) approximate to lambda(-alpha) ; where alpha = angstrom exponent) and averages around 5.2 +/- 2.0 M m(-1) (where M = 10(-6)). A significant decrease in the MAE of BrC from the source region (this study) to the downwind oceanic region (over Bay of Bengal, Srinivas and Sarin, 2013) could be attributed to relative increase in the contribution of non-absorbing WSOC and/or photo-bleaching of BrC during long-range atmospheric transport. The atmospheric radiative forcing due to BrC over the study site accounts for similar to 40% of that from elemental carbon (EC). (C) 2015 Elsevier Ltd. All rights reserved.

Ambient organic carbon (OC) to elemental carbon (EC) ratios are strongly associated with not only the radiative forcing due to aerosols but also the extent of secondary organic aerosol (SOA) formation. An inter-comparison study was conducted based on fine particulate matter samples collected during summer in Beijing to investigate the influence of the thermal-optical temperature protocol on the OC to EC ratio. Five temperature protocols were used such that the NIOSH (National Institute for Occupational Safety and Health) and EUSAAR (European Supersites for Atmospheric Aerosol Research) protocols were run by the Sunset carbon analyzer while the IMPROVE (the Interagency Monitoring of Protected Visual Environments network)-A protocol and two alternative protocols designed based on NIOSH and EUSAAR were run by the DRI analyzer. The optical attenuation measured by the Sunset carbon analyzer was more easily biased by the shadowing effect, whereas total carbon agreed well between the Sunset and DRI analyzers. The ECIMPROVE-A (EC measured by the IMPROVE-A protocol; similar hereinafter) to ECNIOSH ratio and the ECIMPROVE-A to ECEUSAAR ratio averaged 1.36 +/- 0.21 and 0.91 +/- 0.10, respectively, both of which exhibited little dependence on the biomass burning contribution. Though the temperature protocol had substantial influence on the DC to EC ratio, the contributions of secondary organic carbon (SOC) to OC, which were predicted by the EC-tracer method, did not differ significantly among the five protocols. Moreover, the SOC contributions obtained in this study were comparable with previous results based on field observation (typically between 45 and 65%), but were substantially higher than the estimation provided by an air quality model (only 18%). The comparison of SOC and WSOC suggests that when using the transmittance charring correction, all of the three common protocols (i.e., IMPROVE-A, NIOSH and EUSAAR) could be reliable for the estimation of SOC by the EC-tracer method. (C) 2013 Elsevier B.V. All rights reserved.