Summertime oxidative potential of atmospheric PM2.5 over New Delhi: Effect of aerosol ageing.

Exposure to elevated particulate matter (PM) concentrations in ambient air has become a major health concern over urban areas worldwide. Reactive oxygen species (ROS) generation due to ambient PM (termed as their oxidative potential, OP) is shown to play a major role in PM-induced health effects. In the present study, the OP of the ambient PM2.5 samples, collected during summer 2019 from New Delhi, were measured using the dithiothreitol (DTT) assay. Average volume-normalized OP (OPV) was 2.9 ± 1.1 nmol DTT min-1 m-3, and mass-normalized OP (OPm) was 61 ± 29 pmol DTT min-1 µg-1. The regression statistics of OPv vs chemical species show the maximum slope of OPV with the elemental carbon (EC, r2 = 0.72) followed by water-soluble organic carbon (WSOC, r2 = 0.72), and organic carbon (OC, r2 = 0.64). A strong positive correlation between OPm and secondary inorganic aerosols (SIA, such as NH4+ and NO3- mass fractions) was also observed, indicating that the sources emitting NO2 and NH3, precursors of NO3- and NH4+, also emit DTT-active species. Interestingly, the slope value of OPv vs OC for aged aerosols (OM/OC > 1.7, f44 > 0.12 and f43 < 0.04) was 1.7 times higher than relatively fresh organic aerosols (OA, OM/OC < 1.7, f44 < 0.12, f43 > 0.04). An increase in OPv and OPoc with f44 indicates the formation of more DTT active species with the ageing of OA. A linear increase in OPoc with increasing Nitrogen/Carbon (N/C) ratio suggests that nitrogenous OA have higher OP.

Wintertime oxidative potential of PM2.5 over a big urban city in the central Indo-Gangetic Plain.

Indo-Gangetic Plain (IGP) experiences a heavy load of particulate pollution impacting the 9 % of the global population living in this region. The present study examines the dithiothreitol (DTT) assay-based oxidative potential (OP) of PM2.5 and the major sources responsible for the observed OP over the central IGP (Kanpur) during winter. The volume normalized OP (OPV) of PM2.5 varied from 2.7 to 10 nmol DTT min-1 m-3 (5.5 ± 1.5) and mass normalized OP (OPM) of PM2.5 varied from 19 to 58 pmol DTT min-1 µg-1 (34 ± 8.0), respectively. Major sources of PM2.5 were identified using the positive matrix factorization (PMF) and the contribution of these sources to observed OP was estimated through multivariate linear regression of OPv with PMF-resolved factors. Although the PM2.5 mass was dominated by secondary aerosols (SA, 28 %), followed by crustal dust (CD, 24 %), resuspended fine dust (RFD, 14 %), traffic emissions (TE, 8 %), industrial emissions (IE, 17 %), and trash burning (TB, 9 %), their proportionate contribution to OP (except SA) was different likely due to differences in redox properties of chemical species coming from these sources. The SA showed the highest contribution (23 %) to observed OP, followed by RFD (19 %), IE (8 %), TE & TB (5 %), CD (4 %), and others (36 %). Our results highlight the significance of determining the chemical composition of particulates along with their mass concentrations for a better understanding of the relationship between PM and health impacts. Such studies are still lacking in the literature, and these results have direct implications for making better mitigation strategies for healthier air quality.

Aerosol Loading and Radiation Budget Perturbations in Densely Populated and Highly Polluted Indo-Gangetic Plain by COVID-19: Influences on Cloud Properties and Air Temperature.

Aerosols emitted in densely populated and industrialized Indo-Gangetic Plain, one of the most polluted regions in the world, modulate regional climate, monsoon, and Himalayan glacier retreat. Thus, this region is important for understanding aerosol perturbations and their resulting impacts on atmospheric changes during COVID-19 lockdown period, a natural experimental condition created by the pandemic. By analyzing 5 years (2016-2020) data of aerosols and performing a radiative transfer calculation, we found that columnar and near-surface aerosol loadings decreased, leading to reductions in radiative cooling at the surface and top of the atmosphere and atmospheric warming during lockdown period. Further, satellite data analyses showed increases in cloud optical thickness and cloud-particle effective radius and decrease in lower tropospheric air temperature during lockdown period. These results indicate critical influences of COVID-19 lockdown on regional climate and water cycle over Indo-Gangetic Plain, emphasizing need for further studies from modeling perspectives.

Interaction of cesium bound fission product compounds (CsI and CsOH) with abundant inorganic compounds of atmosphere: Effect on hygroscopic growth properties.

Cesium compounds if present in atmosphere, can affect human health as well as the ecosystem due to their highly hazardous nature. Interaction of cesium compounds with abundantly available atmospheric salts can modify the hygroscopic behavior in sub-saturation relative humidity (RH) domain. Any marked modification in growth factor (GF) for the mixed particle state in comparison to the single particles ultimately affects the settling rates and hence the deposition flux. This work studies the hygroscopic behavior of two important cesium bound fission product aerosols (CsI, CsOH) internally mixed with some common atmospheric particles viz. [Formula: see text] and NaNO3 for a fixed dry particle size of 100 nm. Experimental measurements, performed with Hygroscopic tandem differential mobility analyzer in the range of 20-94% RH, have been compared with the predictions made from Zdanovskii-Stokes-Robinson (ZSR) approach. Apart from the single/pure particle state for the constituents (i.e. mixing ratios 1:0 and 0:1), three other mixing ratios 1:4, 1:1 and 4:1 have been considered. The results show that the GF vs RH pattern for mixed particles is different from that for single CsI and CsOH particles. The intrinsic water uptake behavior for these cesium compounds was found to be perturbed for some of the chosen combinations as well. Deliquescent transition for the mixed particles was observed at lower RH compared to the single electrolytes. Relative differences noticeable for the chosen mixing ratios could be related to the available fractions in the mixed state. Overall, ZSR method was found to be capturing the trend of increasing GFs with increasing RH. Terminal gravitational settling velocities calculated from the measured GFs were also found to be different for single and mixed particles. The relative difference was significant for some combinations and test conditions. Any modification in settling velocity ultimately impacts the deposition flux estimations. Hence neglecting the presence of atmospheric salts affects the accuracy of the source term estimates for a postulated nuclear reactor accident scenario.

Diurnal variability in the spectral characteristics and sources of water-soluble brown carbon aerosols over Delhi.

It is well established that light-absorbing organic aerosols (commonly known as brown carbon, BrC) impact climate. However, uncertainties remain as their contributions to absorption at different wavelengths are often ignored in climate models. Further, BrC exhibits differences in absorption at different wavelengths due to the variable composition including varying sources and meteorological conditions. However, diurnal variability in the spectral characteristics of water-soluble BrC (hereafter BrC) is not yet reported. This study presents unique measurement hitherto lacking in the literature. Online measurements of BrC were performed using an assembled system including a particle-into-liquid sampler, portable UV-Visible spectrophotometer with liquid waveguid capillary cell, and total carbon analyzer (PILS-LWCC-TOC). This system measured the absorption of ambient aerosol extracts at the wavelengths ranging from 300 to 600 nm with 2 min integration time and water-soluble organic carbon (WSOC) with 4 min integration time over a polluted megacity, New Delhi. Black carbon, carbon monoxide (CO), nitrogen oxides (NOx), and the chemical composition of non-refractory submicron aerosols were also measured in parallel. Diurnal variability in absorption coefficient (0.05 to 65 Mm-1), mass absorption efficiency (0.01 to 3.4 m-2 gC-1) at 365 nm, and absorption angstrom exponent (AAE) of BrC for different wavelength range (AAE300-400: 4.2-5.8; AAE400-600: 5.5-8.0; and AAE300-600: 5.3-7.3) is discussed. BrC chromophores absorbing at any wavelength showed minimum absorption during afternoon hours, suggesting the effects of boundary layer expansion and their photo-sensitive/volatile nature. On certain days, a considerable presence of BrC absorbing at 490 nm was observed during nighttime that disappears during the daytime. It appeared to be associated with secondary BrC. Observations also infer that BrC species emitted from the biomass and coal burning are more absorbing among all sources. A fraction of BrC is likely associated with trash burning, as inferred from the spectral characteristics of Factor-3 from the PMF analysis of BrC spectra. Such studies are essential in understanding the BrC characteristics and their further utilization in climate models.

Why airborne transmission hasn't been conclusive in case of COVID-19? An atmospheric science perspective.

Airborne transmission is one of the routes for the spread of COVID-19 which is caused by inhalation of smaller droplets1 containing SARS-CoV-2 (i.e., either virus-laden particulate matter: PM and/or droplet nuclei) in an indoor environment. Notably, a significant fraction of the small droplets, along with respiratory droplets, is produced by both symptomatic and asymptomatic individuals during expiratory events such as breathing, sneezing, coughing and speaking. When these small droplets are exposed to the ambient environment, they may interact with PM and may remain suspended in the atmosphere even for several hours. Therefore, it is important to know the fate of these droplets and processes (e.g., physical and chemical) in the atmosphere to better understand airborne transmission. Therefore, we reviewed existing literature focussed on the transmission of SARS-CoV-2 in the spread of COVID-19 and present an environmental perspective on why airborne transmission hasn't been very conclusive so far. In addition, we discuss various environmental factors (e.g., temperature, humidity, etc.) and sampling difficulties, which affect the conclusions of the studies focussed on airborne transmission. One of the reasons for reduced emphasis on airborne transmission could be that the smaller droplets have less number of viruses as compared to larger droplets. Further, smaller droplets can evaporate faster, exposing SARS-CoV-2 within the small droplets to the environment, whose viability may further reduce. For example, these small droplets containing SARS-CoV-2 might also physically combine with or attach to pre-existing PM so that their behaviour and fate may be governed by PM composition. Thus, the measurement of their infectivity and viability is highly uncertain due to a lack of robust sampling system to separately collect virions in the atmosphere. We believe that the present review will help to minimize the gap in our understanding of the current pandemic and develop a robust epidemiological method for mortality assessment.

An application of probability density function for the analysis of PM2.5 concentration during the COVID-19 lockdown period.

The first Covid-19 patient in India was reported on January 30, 2020 at the state of Kerala. The patient number rose to three by February 3, 2020. In the month of March 2020, the transmissions started to increase when the people started to return back to India from the Covid-19 affected countries. On March 12, a 76-year-old man having a travel history to Saudi Arabia was the first reported fatality in India due to Covid 19. Then for the prevention of the propagation of Covid, the Indian government declared a state of health emergency and strict counter measures were taken, including locking down of cities, prohibiting almost all avoidable activities and restricting population's mobility. From March 24, 2020 due to the complete lockdown in the country, human activities were heavily restricted in the whole geographical regions of India. This pandemic lockdown eventually serves as an opportunity to observe the background concentrations of pollutants in the atmosphere. The PM 2.5 distribution can affect human health and to overcome this problem, setting up of regulation for PM is necessary. In the present study Probability density functions (PDF) method have been utilised for the investigation of PM 2.5 pollutant data distribution of five countries namely, India, China, France, Brazil and United States of America (USA) for their respective lockdown period of 2020 and corresponding same period of 2019. A detailed study has been done for India, and for that purpose India has been divided into three regions (Central India, Coastal India and Indo-Gangetic Plain (IGP)) on the basis of different meteorological conditions. PM 2.5 concentration for hourly basis has been analysed for the lockdown period 24th March to 15th June 2020 and compared with the PM 2.5 concentration of previous year 2019 for the same time period. To understand the effect of lockdown in PM 2.5 emission in India, which will give us an idea about the background concentration, PDFs (probability density functions) have also been generated for the whole year from 2015 to 2019. The "goodness-of-fit" of the probability density functions, to the data, was assessed, using various statistical indices (Chi-square test). Results show that the PM 2.5 reduction during the lockdown period of 2020 as compared to the same period of 2019 is sufficiently large. This study will give a certain degree of idea to the regulatory bodies on planning and implementation of strict air quality control plans.

Large global variations in measured airborne metal concentrations driven by anthropogenic sources.

Globally consistent measurements of airborne metal concentrations in fine particulate matter (PM2.5) are important for understanding potential health impacts, prioritizing air pollution mitigation strategies, and enabling global chemical transport model development. PM2.5 filter samples (N ~ 800 from 19 locations) collected from a globally distributed surface particulate matter sampling network (SPARTAN) between January 2013 and April 2019 were analyzed for particulate mass and trace metals content. Metal concentrations exhibited pronounced spatial variation, primarily driven by anthropogenic activities. PM2.5 levels of lead, arsenic, chromium, and zinc were significantly enriched at some locations by factors of 100-3000 compared to crustal concentrations. Levels of metals in PM2.5 and PM10 exceeded health guidelines at multiple sites. For example, Dhaka and Kanpur sites exceeded the US National Ambient Air 3-month Quality Standard for lead (150 ng m-3). Kanpur, Hanoi, Beijing and Dhaka sites had annual mean arsenic concentrations that approached or exceeded the World Health Organization's risk level for arsenic (6.6 ng m-3). The high concentrations of several potentially harmful metals in densely populated cites worldwide motivates expanded measurements and analyses.

Wintertime hygroscopic growth factors (HGFs) of accumulation mode particles and their linkage to chemical composition in a heavily polluted urban atmosphere of Kanpur at the Centre of IGP, India: Impact of ambient relative humidity.

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.

Realtime chemical characterization of post monsoon organic aerosols in a polluted urban city: Sources, composition, and comparison with other seasons.

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.

Refractive Index and Absorption Attribution of Highly Absorbing Brown Carbon Aerosols from an Urban Indian City-Kanpur.

Atmospheric aerosols influence Earth's radiative balance, having both warming and cooling effects. Though many aerosols reflect radiation, carbonaceous aerosols such as black carbon and certain organic carbon species known as brown carbon have the potential to warm the atmosphere by absorbing light. Black carbon absorbs light over the entire solar spectrum whereas brown carbon absorbs near-UV wavelengths and, to a lesser extent, visible light. In developing countries, such as India, where combustion sources are prolific, the influence of brown carbon on absorption may be significant. In order to better characterize brown carbon, we present experimental and modeled absorption properties of submicron aerosols measured in an urban Indian city (Kanpur). Brown carbon here is found to be fivefold more absorbing at 365 nm wavelength compared to previous studies. Results suggest ~30% of total absorption in Kanpur is attributed to brown carbon, with primary organic aerosols contributing more than secondary organics. We report the spectral brown carbon refractive indices along with an experimentally constrained estimate of the influence of aerosol mixing state on absorption. We conclude that brown carbon in Kanpur is highly absorbing in nature and that the mixing state plays an important role in light absorption from volatile species.

Highly time resolved chemical characterization of submicron organic aerosols at a polluted urban location.

Non-refractory submicron (NR-PM1) aerosols were measured during the late winter period (February-March) via an Aerodyne High Resolution Time of Flight Aerosols Mass Spectrometer (HR-ToF-AMS) along with Black Carbon (BC) and trace gasses in an industrial city, Kanpur, situated in the Gangetic Plain (GP) of India. The composition of NR-PM1 aerosols was dominated by organics (54%), followed by inorganics (36%), and BC (10%). Source apportionment via Positive Matrix Factorization (PMF) of AMS measured organic aerosols (OAs) revealed 6 factors. Factors are identified as 2 types of oxidized organic aerosols (OOAs), 2 types of biomass burning organic aerosols (BBOAs), freshly emitted hydrocarbon-like organic aerosols (HOAs) and oxygenated primary organic aerosols (OPOAs). A substantial increase in relative OOA contributions (200%) and O/C ratio (26%) has been observed from the high loading events (HLE) to the low loading events (LLE). Back trajectory analysis indicated that the study location received contributions from regional and long-range transported aerosols. OA composition and evolution during this study period were also very different from those observed during a fog influenced peak winter period of December-January. This is the first study to present detailed aerosol composition during the late winter period in India highlighting the changes in OA composition and chemistry within the same winter season.

Combined effects of organic aerosol loading and fog processing on organic aerosols oxidation, composition, and evolution.

Chemical characterization of ambient non-refractory submicron aerosols (NR-PM1) was carried out in real time at Kanpur, India. The measurements were performed during the winter (December 2014 to February 2015), and comprised of two very distinct high and low aerosol loading periods coupled with prevalent foggy conditions. The average non-refractory submicron aerosol loading varied significantly from high (HL, ~240µg/m3) to low loading (LL, ~100µg/m3) period and was dominated by organic aerosols (OA) which contributed more than half (~60%) of the measured aerosol mass. OA source apportionment via positive matrix factorization (PMF) showed drastic changes in the composition of OA from HL to LL period. Overall, O/C (oxygen to carbon) ratios also varied significantly from HL (=0.59) to LL (=0.69) period. Fog episodes (n=17) studied here seem to be reducing the magnitude of the negative impact of OA loading on O/C ratio (OA loading and O/C ratio are anti-correlated, as higher OA loading allows gas to particle partitioning of relatively less oxidized organics) by 60% via aqueous processing. This study provided new insights into the combined effects of OA loading and fog aqueous processing on the evolution of ambient organic aerosols (OA) for the first time.

Contribution of Brown Carbon to Direct Radiative Forcing over the Indo-Gangetic Plain.

The Indo-Gangetic Plain is a region of known high aerosol loading with substantial amounts of carbonaceous aerosols from a variety of sources, often dominated by biomass burning. Although black carbon has been shown to play an important role in the absorption of solar energy and hence direct radiative forcing (DRF), little is known regarding the influence of light absorbing brown carbon (BrC) on the radiative balance in the region. With this in mind, a study was conducted for a one month period during the winter-spring season of 2013 in Kanpur, India that measured aerosol chemical and physical properties that were used to estimate the sources of carbonaceous aerosols, as well as parameters necessary to estimate direct forcing by aerosols and the contribution of BrC absorption to the atmospheric energy balance. Positive matrix factorization analyses, based on aerosol mass spectrometer measurements, resolved organic carbon into four factors including low-volatile oxygenated organic aerosols, semivolatile oxygenated organic aerosols, biomass burning, and hydrocarbon like organic aerosols. Three-wavelength absorption and scattering coefficient measurements from a Photo Acoustic Soot Spectrometer were used to estimate aerosol optical properties and estimate the relative contribution of BrC to atmospheric absorption. Mean ± standard deviation values of short-wave cloud free clear sky DRF exerted by total aerosols at the top of atmosphere, surface and within the atmospheric column are -6.1 ± 3.2, -31.6 ± 11, and 25.5 ± 10.2 W/m(2), respectively. During days dominated by biomass burning the absorption of solar energy by aerosols within the atmosphere increased by ∼35%, accompanied by a 25% increase in negative surface DRF. DRF at the top of atmosphere during biomass burning days decreased in negative magnitude by several W/m(2) due to enhanced atmospheric absorption by biomass aerosols, including BrC. The contribution of BrC to atmospheric absorption is estimated to range from on average 2.6 W/m(2) for typical ambient conditions to 3.6 W/m(2) during biomass burning days. This suggests that BrC accounts for 10-15% of the total aerosol absorption in the atmosphere, indicating that BrC likely plays an important role in surface and boundary temperature as well as climate.

The discoloration of the Taj Mahal due to particulate carbon and dust deposition.

The white marble domes of the Taj Mahal are iconic images of India that attract millions of visitors every year. Over the past several decades the outer marble surfaces of the Taj Mahal have begun to discolor with time and must be painstakingly cleaned every several years. Although it has been generally believed that the discoloration is in some way linked with poor air quality in the Agra region, the specific components of air pollution responsible have yet to be identified. With this in mind, ambient particulate matter (PM) samples were collected over a one-year period and found to contain relatively high concentrations of light absorbing particles that could potentially discolor the Taj Mahal marble surfaces, that include black carbon (BC), light absorbing organic carbon (brown carbon, BrC), and dust. Analyses of particles deposited to marble surrogate surfaces at the Taj Mahal indicate that a large fraction of the outer Taj Mahal surfaces are covered with particles that contain both carbonaceous components and dust. We have developed a novel approach that estimates the impact of these deposited particles on the visible light surface reflectance, which is in turn used to estimate the perceived color by the human eye. Results indicate that deposited light absorbing dust and carbonaceous particles (both BC and BrC from the combustion of fossil fuels and biomass) are responsible for the surface discoloration of the Taj Mahal. Overall, the results suggest that the deposition of light absorbing particulate matter in regions of high aerosol loading are not only influencing cultural heritage but also the aesthetics of both natural and urban surfaces.

Measurement of personal and integrated exposure to particulate matter and co-pollutant gases: a panel study.

Personal exposure measurement can serve as an effective tool to understand the effect of exposure to air pollutants. Alternatively, exposure assessment using pollutant concentrations in different microenvironments and accurate time-activity information for the subjects can provide good information regarding human integrated exposure. A panel of 18 healthy students of Indian Institute of Technology (IIT) Kanpur in the age group of 18 to 30 years participated in the personal exposure measurements for particulate matter, CO, NO(2) and VOC during post-monsoon and pre-monsoon seasons. Overall, 432 h person exposure data was collected in this study. The major sources of particulate and gaseous co-pollutants were identified. These directly obtained personal exposure values were then compared to the indirectly estimated integrated exposure values. Personal and integrated exposures gave statistically similar results. Through this study, we have shown that integrated exposure values could closely estimate the personal exposure values for particulate matter that can significantly reduce time and cost involved in personal exposure studies. The lung parameters for all the subjects measured during the pre-monsoon and post-monsoon seasons showed statistically significant reduction during pre-monsoon. This was attributed to the high levels of coarse particles during pre-monsoon.

Comparison of experimental and modeled absorption enhancement by black carbon (BC) cored polydisperse aerosols under hygroscopic conditions.

The quantification of the radiative impacts of light absorbing ambient black carbon (BC) particles strongly depends on accurate measurements of BC mass concentration and absorption coefficient (ß(abs)). In this study, an experiment has been conducted to quantify the influence of hygroscopic growth of ambient particles on light absorption. Using the hygroscopic growth factor (i.e., Zdanovskii-Stokes-Robinson (ZSR) approach), a model has been developed to predict the chemical composition of particles based on measurements, and the absorption and scattering coefficients are derived using a core-shell assumption with light extinction estimates based on Mie theory. The estimated optical properties agree within 7% for absorption coefficient and 30% for scattering coefficient with that of measured values. The enhancement of absorption is found to vary according to the thickness of the shell and BC mass, with a maximum of 2.3 for a shell thickness of 18 nm for the particles. The findings of this study underline the importance of considering aerosol-mixing states while calculating their radiative forcing.

Temporal trends in atmospheric PM2.5, PM10, elemental carbon, organic carbon, water-soluble organic carbon, and optical properties: impact of biomass burning emissions in the Indo-Gangetic Plain.

The first simultaneous measurements and analytical data on atmospheric concentrations of PM(2.5), PM(10), inorganic constituents, carbonaceous species, and their optical properties (aerosol optical depth, AOD; absorption coefficient, b(abs); mass absorption efficiency, σ(abs); and single scattering albedo, SSA) from an urban site (Kanpur) in the Indo-Gangetic Plain are reported here. Significantly high aerosol mass concentration (>100 µg m(-3)) and AOD (> 0.3) are seen as a characteristic feature throughout the sampling period, from October 2008 to April 2009. The temporal variability in the mass fractions of carbonaceous species (EC, OC, and WSOC) is pronounced during October-January when emissions from biomass burning are dominant and OC is a major constituent (∼30%) of PM(2.5) mass. The WSOC/OC ratio varies from 0.21 to 0.65, suggesting significant contribution from secondary organic aerosols (SOAs). The mass fraction of SO(4)(2-) in PM(2.5) (Av: 12.5%) exceeds that of NO(3)(-) and NH(4)(+). Aerosol absorption coefficient (@ 678 nm) decreases from 90 Mm(-1) (in December) to 20 Mm(-1) (in April), and a linear regression analysis of the data for b(abs) and EC (n = 54) provides a measure of the mass absorption efficiency of EC (9.6 m(2) g(-1)). In contrast, scattering coefficient (@ 678 nm) increases from 98 Mm(-1) (in January) to 1056 Mm(-1) (in April) and an average mass scattering efficiency of 3.0 ± 0.9 m(2) g(-1) is obtained for PM(10) samples. The highest b(scat) was associated with the dust storm event (April 17, 2009) over northern Iraq, eastern Syria, and southern Turkey; thus, resulting in high SSA (0.93 ± 0.02) during March-April compared to 0.82 ± 0.04 in October-February. These results have implications to large temporal variability in the atmospheric radiative forcing due to aerosols over northern India.

Secondary organic aerosol: a comparison between foggy and nonfoggy days.

Carbonaceous species, meteorological parameters, trace gases, and fogwater chemistry were measured during winter in the Indian city of Kanpur to study secondary organic aerosol (SOA) during foggy and clear (nonfoggy) days. Enhanced SOA production was observed during fog episodes. It is hypothesized that aqueous phase chemistry in fog drops is responsible for increasing SOA production. SOA concentrations on foggy days exceeded those on clear days at all times of day; peak foggy day SOA concentrations were observed in the evening vs peak clear day SOA concentrations which occurred in the afternoon. Changes in biomass burning emissions on foggy days were examined because of their potential to confound estimates of SOA production based on analysis of organic to elemental carbon (OC/EC) ratios. No evidence of biomass burning influence on SOA during foggy days was found. Enhanced oxidation of SO(2) to sulfate during foggy days was observed, possibly causing the regional aerosol to become more acidic. No evidence was found in this study, either, for effects of temperature or relative humidity on SOA production. In addition to SOA production, fogs can also play an important role in cleaning the atmosphere of carbonaceous aerosols. Preferential scavenging of water-soluble organic carbon (WSOC) by fog droplets was observed. OC was found to be enriched in smaller droplets, limiting the rate of OC deposition by droplet sedimentation. Lower EC concentrations were observed on foggy days, despite greater stagnation and lower mixing heights, suggesting fog scavenging and removal of EC was active as well.