ABSTRACT
Atmospheric brown carbon (BrC), a short-lived climate forcer, absorbs solar radiation and is a substantial contributor to the warming of the Earth's atmosphere. BrC composition, its absorption properties, and their evolution are poorly represented in climate models, especially during atmospheric aqueous events such as fog and clouds. These aqueous events, especially fog, are quite prevalent during wintertime in Indo-Gangetic Plain (IGP) and involve several stages (e.g., activation, formation, and dissipation, etc.), resulting in a large variation of relative humidity (RH) in the atmosphere. The huge RH variability allowed us to examine the evolution of water-soluble brown carbon (WS-BrC) diurnally and as a function of aerosol liquid water content (ALWC) and RH in this study. We explored links between the evolution of WS-BrC mass absorption efficiency at 365 nm (MAEWS-BrC-365) and chemical characteristics, viz., low-volatility organics and water-soluble organic nitrogen (WSON) to water-soluble organic carbon (WSOC) ratio (org-N/C), in the field (at Kanpur in central IGP) for the first time worldwide. We observed that WSON formation governed enhancement in MAEWS-BrC-365 diurnally (except during the afternoon) in the IGP. During the afternoon, the WS-BrC photochemical bleaching dwarfed the absorption enhancement caused by WSON formation. Further, both MAEWS-BrC-365 and org-N/C ratio increased with a decrease in ALWC and RH in this study, signifying that evaporation of fog droplets or bulk aerosol particles accelerated the formation of nitrogen-containing organic chromophores, resulting in the enhancement of WS-BrC absorptivity. The direct radiative forcing of WS-BrC relative to that of elemental carbon (EC) was â¼19 % during wintertime in Kanpur, and â¼ 40 % of this contribution was in the UV-region. These findings highlight the importance of further examining the links between the evolution of BrC absorption behavior and chemical composition in the field and incorporating it in the BrC framework of climate models to constrain the predictions.
ABSTRACT
This study reported results of the wintertime simultaneous measurements of hygroscopic growth factors (HGFs) and particle-phase chemical composition of accumulation mode particles using a self-assembled Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA) and an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS), respectively at a heavily polluted urban atmosphere of Kanpur, situated in the center of IGP in India. HGFs at 85% relative humidity (RH) and the size-resolved composition of ambient aerosol particles (dry electrical mobility diameters of 100 and 150 nm) were investigated. HGF_85% was found to increase with particle size. The relative mass fraction of organic aerosol (OA) and NH4NO3 are probably the major contributors to the fluctuation of the HGF_85% for both particle sizes. The HGF_85% of accumulation mode particles were observed to increase from the minimum value observed during the morning until its maximum afternoon value. This study reported two maximum (early morning and afternoon time) and two minimum values (morning and evening time) of HGF_85%s. As a consequence, the main reasons for this incremental behavior were, increase in the ratio of inorganic to OA and oxidation level, f44 (m/z44/OA) of the OA within the particle phase. In context to the effect of ambient RH, this study reported two distinct variations of mean HGF_85% as the function of ambient RH. The positive linear relationship at low RH (LRH, RH ≤ 50%) was clearly associated with low OA loading, relatively higher substantial temperature, and wind speed. We also observed increment in f44, and effective density indicating aging of aerosol. However, HGF_85% was found to inversely decline as a function of RH at higher RH (HRH, RH > 50%) conditions, which clearly reflect the more significant contribution of primary OA and lower oxidation level of OA. Our results show the declining trend in size-resolved effective density at HRH conditions, confirming the above conclusions.
ABSTRACT
Real time chemical characterization of non-refractory submicron aerosols (NR-PM1) was carried out during post monsoon (September-October) via Aerosol Mass Spectrometer (AMS) at a polluted urban location of Kanpur, India. Organic aerosol (OA) was found to be the dominant species with 58% contribution to total NR-PM1 mass, followed by sulfate (16%). Overall, OA was highly oxidized (average O/C = 0.66) with the dominance of oxidized OAs (60% of total OA) as revealed by source apportionment. Oxidized nature of OA was also supported by very high OC/EC ratios (average = 8.2) obtained from simultaneous offline filter sampling. High and low OA loading periods have very dramatic effects on OA composition and oxidation. OA O/C ratios during lower OA loading periods were on average 30% higher than the same from high loading periods with significant changes in types and relative contribution from oxidized OAs (OOA). Comparison of OA sources and chemistry among post monsoon and other seasons revealed significant differences. Characteristics of primary OAs remain very similar, but features of OOAs showed substantial changes from one season to another. Winter had lowest OOA contribution to total OA but similar overall O/C ratios as other seasons. This reveals that processing of primary OAs, local atmospheric chemistry, and regional contributions can significantly alter OA characteristics from one season to another. This study provides interesting insights into the seasonal variations of OA sources and evolution in a very polluted and complex environment.
