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In this paper, we synthesize the size distribution and optical properties of the atmospheric water-soluble fraction of light-absorbing organic carbon (brown carbon; BrC) in the continental outflow from the Indo-Gangetic Plain (IGP) in South Asia to the North Indian Ocean. A comparison of the mass absorption coefficient of water-soluble BrC (babs-WSBrC-365nm) in PM2.5 with that in PM10 sampled over the Bay of Bengal reveals the dominance of BrC in fine mode. Furthermore, the babs-BrC-365nm shows a significant linear relationship with mass concentrations of airborne particulate matter, water-soluble organic carbon and non-sea-salt-K+ in the continental outflow from the IGP. This observation emphasizes the ubiquitous nature and significant contribution of water-soluble BrC from biomass burning emissions (BBEs). Comparing the absorption properties from this study with global datasets, it is discernible that BBEs dominate BrC absorption. Furthermore, the imaginary refractive index of water-soluble BrC (kWSBrC-365nm) in marine aerosols sampled over the North Indian Ocean during November is significantly higher than during December to January. Thus, significant temporal variability is associated with crop-residue burning emissions in the IGP on the composition of BrC over the North Indian Ocean. Our estimates show that the babs-WSBrC-365nm and kWSBrC-365nm from post-harvest crop-residue burning emissions in the IGP are much higher than the BBEs from the southeastern United States and Amazonian forest fires. Another major finding of this study is the lack of significant relationship between kWSBrC-365nm and the mass ratio of elemental carbon to particulate organic matter, as previously suggested by chamber experiments to model varying BrC absorption properties in ambient aerosols. Therefore, considerable spatio-temporal variability prevails among emission sources (wood burning vs. crop-residue burning), which needs to be considered when assessing the regional radiative forcing of BrC relative to major absorbing elemental carbon.

A lack of consensus on the distributions and formation pathways of secondary organic aerosols (SOA) over oceanic regions downwind of pollution sources limits our ability to assess their climate impact globally. As a case study, we report here on water-soluble SOA components such as dicarboxylic acids, oxocarboxylic acids, and α-dicarbonyls in the continental outflows from the Indo-Gangetic Plain (IGP) and Southeast Asia (SEA) to the Bay of Bengal. Oxalic acid (C 2 ) is the dominant species followed by succinic (C 4 ) and glyoxylic acids (ωC 2 ) in the outflow. Nonsea-salt SO 4 2- also dominates (∼70%) total water-soluble inorganic constituents and correlates well with aerosol liquid water content (LWC) and C 2 , indicating their production through aqueous phase photochemical reactions. Furthermore, mass ratios of dicarboxylic acids (C 2 /C 4 , C 2 /ωC 2 ), and their relative abundances in water-soluble organic carbon and total organic carbon are quite similar between the two continental (IGP and SEA) outflows, indicating the formation of SOA through aqueous phase photochemical reactions in LWC-enriched aerosols, largely controlled by anthropogenic SO 4 2- .

In the present-day scenario of growing anthropogenic activities, carbonaceous aerosols contribute significantly (∼20-70%) to the total atmospheric particulate matter mass and, thus, have immense potential to influence the Earth's radiation budget and climate on a regional to global scale. In addition, formation of secondary organic aerosols is being increasingly recognized as an important process in contributing to the air-pollution and poor visibility over urban regions. It is, thus, essential to study atmospheric concentrations of carbonaceous species (EC, OC and WSOC), their mixing state and absorption properties on a regional scale. This paper presents the comprehensive data on emission sources, chemical characteristics and optical properties of carbonaceous aerosols from selected urban sites in the Indo-Gangetic Plain (IGP) and from a high-altitude location in the central Himalaya. The mass concentrations of OC, EC and WSOC exhibit large spatio-temporal variability in the IGP. This is attributed to seasonally varying emissions from post-harvest agricultural-waste burning, their source strength, boundary layer dynamics and secondary aerosol formation. The high concentrations of OC and SO4(2-), and their characteristic high mass scattering efficiency, contribute significantly to the aerosol optical depth and scattering coefficient. This has implications to the assessment of single scattering albedo and aerosol radiative forcing on a regional scale., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

Temporal variability (November'09-March'10) in the mass concentrations of PM2.5, mineral dust, organic carbon and elemental carbon (OC and EC), water-soluble organic carbon (WSOC) and inorganic species (WSIS) has been studied in the atmospheric outflow to the Bay of Bengal from a sampling site [Kharagpur: 22.02°N, 87.11°E] in the Indo-Gangetic Plain (IGP). Based on diagnostic ratios of carbonaceous species [OC/EC ≈ 7.0 ± 2.2, WSOC/OC ≈ 0.52 ± 0.16, and K(+)/EC≈0.48±0.17], we document dominant impact from biomass burning emissions (wood-fuel and post-harvest agricultural-waste burning) in the IGP-outflow. Relatively high concentration of sulphate (SO4(2-) ≈ 6.9-25.3 μg m(-3); SO4(2-)/ΣWSIS=45-77%) and characteristic ratios of nss-SO4(2-)/EC (3.9 ± 2.1) and nss-SO4(2-)/OC (0.61 ± 0.46) provide information on absorption/scattering properties of aerosols. Based on quantitative assessment of individual components of PM2.5, we document aerosol organic carbon-to-organic mass (OC to OM) conversion factor centring at 1.5 ± 0.2 (range: 1.3-2.7) in the atmospheric outflow from IGP. The aerosol composition over the Bay of Bengal shows striking similarity with the diagnostic ratios documented for the IGP-outflow. Relatively high conversion factor for assessing the mass of organic aerosols over the Bay of Bengal (1.1-3.7) provides evidence for their oxidation during long-range atmospheric transport., (Copyright © 2014 Elsevier B.V. All rights reserved.)

Emission from large-scale post-harvest agricultural-waste burning (paddy-residue burning during October-November and wheat-residue burning in April-May) is a conspicuous feature in northern India. The poor and open burning of agricultural residue result in massive emission of carbonaceous aerosols and organic pollutants to the atmosphere. In this context, concentrations of atmospheric polycyclic aromatic hydrocarbons (PAHs) and their isomer ratios have been studied for a 2-year period from a source region (Patiala: 30.2°N; 76.3°E) of two distinct biomass burning emissions. The concentrations of 4-6 ring PAHs are considerably higher compared to 2-3 ring PAHs in the ambient particulate matter (PM2.5). The crossplots of PAH isomer ratios, fluoranthene / (fluoranthene + pyrene) and indeno[1,2,3-cd]pyrene/(indeno[1,2,3-cd]pyrene + benzo[g,h,i]perylene) for two biomass burning emissions, exhibit distinctly different source characteristics compared to those for fossil-fuel combustion sources in south and south-east Asia. The PAH isomer ratios studied from different geographical locations in northern India also exhibit similar characteristics on the crossplot, suggesting their usefulness as diagnostic tracers of biomass burning emissions.

Atmospheric PM2.5 (particulate matter with aerodynamic diameter of ≤ 2.5 μm), collected from a source region [Patiala: 30.2 °N; 76.3 °E; 250 m above mean sea level] of emissions from post-harvest agricultural-waste (paddy-residue) burning in the Indo-Gangetic Plain (IGP), North India, has been studied for its chemical composition and impact on regional atmospheric radiative forcing. On average, organic aerosol mass accounts for 63% of PM2.5, whereas the contribution of elemental carbon (EC) is ∼3.5%. Sulphate, nitrate and ammonium contribute up to ∼85% of the total water-soluble inorganic species (WSIS), which constitutes ∼23% of PM2.5. The potassium-to-organic carbon ratio from paddy-residue burning emissions (KBB(+)/OC: 0.05 ± 0.01) is quite similar to that reported from Amazonian and Savanna forest-fires; whereas non-sea-salt-sulphate-to-OC ratio (nss-SO4(2-)/OC: 0.21) and nss-SO4(2-)/EC ratio of 2.6 are significantly higher (by factor of 5 to 8). The mass absorption efficiency of EC (3.8 ± 1.3 m(2) g(-1)) shows significant decrease with a parallel increase in the concentrations of organic aerosols and scattering species (sulphate and nitrate). A cross plot of OC/EC and nss-SO4(2-)/EC ratios show distinct differences for post-harvest burning emissions from paddy-residue as compared to those from fossil-fuel combustion sources in south-east Asia.

A systematic study on the chemical characteristics of ambient PM2.5, collected during October-2011 to March-2012 from a source region (Patiala: 30.2°N, 76.3°E; 250 m amsl) of biomass burning emissions in the Indo-Gangetic Plain (IGP), exhibit pronounced diurnal variability in mass concentrations of PM2.5, NO3(-), NH4(+), K(+), OC, and EC with ~30-300% higher concentrations in the nighttime samples. The average WSOC/OC and SO4(2-)/PM2.5 ratios for the daytime (~0.65, and 0.18, respectively) and nighttime (0.45, and 0.12, respectively) samples provide evidence for secondary organic and SO4(2-) aerosol formation during the daytime. Formation of secondary NO3(-) is also evident from higher NH4NO3 concentrations associated with lower temperature and higher relative humidity conditions. The scattering species (SO4(2-) + NO3(-) + OC) contribute ~50% to PM2.5 mass during October-March whereas absorbing species (EC) contribute only ~4% in October-February and subsequently increases to ~10% in March, indicating significance of these species in regional radiative forcing., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

This study presents the first data set on atmospheric input of N, P and Fe to the Northern Indian Ocean. Based on the chemical analysis of ambient aerosols, collected from the marine atmospheric boundary layer (MABL) during the continental outflow (January-April), we document that dry-deposition fluxes (μmolm(-2) d(-1)) of N (2-167), P (0.5-4.8) and Fe (0.02-1.2) to the Bay of Bengal are significantly higher compared to those over the Arabian Sea [N: 0.2-18.6; P: 0.3-0.9; Fe: 0.001-0.015]. Using atmospherically derived P and Fe, C-fixation (1.1 Pg yr(-1)) in the Bay of Bengal is dominated by anthropogenic sources. In contrast, C-fixation (0.03 Pg yr(-1)) in the Arabian Sea is limited by P and Fe. This is attributed to the poor fractional solubility of atmospheric mineral dust transported to the Arabian Sea. However, N-fixation by diazotrophs in the two oceanic regions is somewhat similar (0.5 Tg yr(-1)). Our estimate of N-deposition (0.2 Tg yr(-1)) to the Northern Indian Ocean is significantly lower compared to model results (~800-1200 mg-Nm(-2)yr(-1)≈5.7-8.6 Tg yr(-1) by Duce et al. (2008); ~4.1 Tg yr(-1) by Okin et al. (2011); ~0.8 Tg yr(-1) by Kanakidou et al. (2012)). An overestimate of N-deposition by models could arise due to inappropriate parameterization of temporal variability associated with the continental outflow spread over only four months., (Copyright © 2013 Elsevier B.V. All rights reserved.)