Kirpa Ram

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.

Absorption Coefficient and Site-Specific Mass Absorption Efficiency of Elemental Carbon in Aerosols over Urban, Rural, and High-Altitude Sites in India

Temporal and spatial variability in the absorption coefficient (b(abs), Mm(-1)) and mass absorption efficiency (MAE, sigma(abs), m(2)g(-1)) of elemental carbon (EC) in atmospheric aerosols studied from urban, rural, and high-altitude sites is reported here. Ambient aerosols, collected on tissuquartz filters, are analyzed for EC mass concentration using thermo-optical EC-OC analyzer, wherein simultaneously measured optical-attenuation (ATN, equivalent to initial transmittance) of 678 nm laser source has been used for the determination of MAE and absorption coefficient. At high-altitude sites, measured ATN and surface EC loading (EC(s), microg cm(-2)) on the filters exhibit linear positive relationship (R(2) = 0.86-0.96), suggesting EC as a principal absorbing component. However, relatively large scatter in regression analyses for the data from urban sites suggests contribution from other species. The representative MAE of EC, during wintertime (Dec 2004), at a rural site (Jaduguda) is 6.1 +/- 2.0 m(2)g(-1). In contrast, MAE at the two high-altitude sites is 14.5 +/- 1.1 (Manora Peak) and 10.4 +/- 1.4 (Mt. Abu); and that at urban sites is 11.1 +/- 2.6 (Allahabad) and 11.3 +/- 2.2 m(2)g(-1) (Hisar). The long-term average MAE at Manora Peak (February 2005 to June 2007) is 12.8 +/- 2.9 m(2)g(-1) (range: 6.1-19.1 m(2)g(-1)). These results are unlike the constant conversion factor used for MAE in optical instruments for the determination of BC mass concentration. The absorption coefficient also shows large spatiotemporal variability; the lower values are typical of the high-altitude sites and higher values for the urban and rural atmosphere. Such large variability documented for the absorption parameters suggests the need for their suitable parametrization in the assessment of direct aerosol radiative forcing on a regional scale.

Atmospheric carbonaceous aerosols from Indo-Gangetic Plain and Central Himalaya: Impact of anthropogenic sources

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 Earths 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.

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 (β(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.

Aerosol optical properties and radiative effects over Manora Peak in the Himalayan foothills: seasonal variability and role of transported aerosols

The higher altitude regions of Himalayas and Tibetan Plateau are influenced by the dust and black carbon (BC) aerosols from the emissions and long-range transport from the adjoining areas. In this study, we present impacts of advection of polluted air masses of natural and anthropogenic emissions, on aerosol optical and radiative properties at Manora Peak (~2000 m amsl) in central Himalaya over a period of more than two years (February 2006-May 2008). We used the most updated and comprehensive data of chemical and optical properties available in one of the most climatically sensitive region, the Himalaya, to estimate atmospheric radiative forcing and heating rate. Aerosol optical depth (AOD) was found to vary from 0.04 to 0.45 with significantly higher values in summer mainly due to an increase in mineral dust and biomass burning aerosols due to transport. In contrast, single scattering albedo (SSA) varied from 0.74 to 0.88 with relatively lower values during summer, suggesting an increase in absorbing BC and mineral dust aerosols. As a result, a large positive atmospheric radiative forcing (about 28 ± 5 Wm(-2)) and high values of corresponding heating rate (0.80 ± 0.14 Kday(-1)) has been found during summer. During the entire observation period, radiative forcing at the top of the atmosphere varied from -2 to +14 Wm(-2) and from -3 to -50 Wm(-2) at the surface whereas atmospheric forcing was in the range of 3 to 65 Wm(-2) resulting in a heating rate of 0.1-1.8 Kday(-1).

Atmospheric 210Pb, 210Po and 210Po/210Pb activity ratio in urban aerosols: temporal variability and impact of biomass burning emission

ABSTRACT Atmospheric 210Pb, 210Po and their activity ratio (210Po/210Pb) have been studied for two years (January 2007–April 2009) from an urban site (Kanpur: 26.5°N and 80.3°E) in the Indo-Gangetic Plain. The average activities of 210Pb and 210Po centre on 1.8 mBq m−3 (range: 0.5–4.8 mBq m−3 for n=99) and 0.094 mBq m−3 (n=21, range: 0.002–0.28 mBq m−3), respectively. The temporal variability in the activity of 210Pb is significantly pronounced, with relatively high levels during October–November and December–February; a trend similar to that observed for the carbonaceous species. The high aerosol abundance coinciding with the biomass burning emissions (agricultural-waste burning) during October–November and stagnant boundary layer in the wintertime (December–February) is the dominant factor for the observed temporal trend. The preliminary data suggest that biomass burning emissions also contribute to the atmospheric 210Po activity, as evident from the large variability in the 210Po/210Pb activity ratio (range: 0.02–0.23) at this urban site. These results have implications to the model-based activity levels of 210Pb and 210Po from in-situ decay of the parent nuclide (222Rn) for given latitude. †Now at: Department of Earth and Planetary Science, Graduate School of Science, University of Tokyo, Tokyo, Japan.

Dual‐carbon‐isotope characterization of total organic carbon in wintertime carbonaceous aerosols from northern India

Large-scale emissions of carbonaceous aerosols (CA) from South Asia impact both regional climate and air quality, yet their sources are not well constrained. Here we use source-diagnostic stable an ...

Humic-Like Substances (HULIS) in Aerosols of Central Tibetan Plateau (Nam Co, 4730 m asl): Abundance, Light Absorption Properties, and Sources

Humic-like substances (HULIS) are major components of light-absorbing brown carbon that play an important role in Earths radiative balance. However, their concentration, optical properties, and sources are least understood over Tibetan Plateau (TP). In this study, the analysis of total suspended particulate (TSP) samples from central of TP (i.e., Nam Co) reveal that atmospheric HULIS are more abundant in summer than that in winter without obvious diurnal variations. The light absorption ability of HULIS in winter is 2-3 times higher than that in summer. In winter, HULIS are mainly derived from biomass burning emissions in South Asia by long-range transport. In contrast, the oxidation of anthropogenic and biogenic precursors from northeast part of India and southeast of TP are major sources of HULIS in summer.

Exploring the relationship between surface PM 2.5 and meteorology in Northern India

Northern India (23–31 N, 68–90 E) is one of the most densely populated and polluted regions in world. Accurately modeling pollution in the region is difficult due to the extreme conditions with respect to emissions, meteorology, and topography, but it is paramount in order to understand how future changes in emissions and climate may alter the region’s pollution regime. We evaluate the ability of a developmental version of the new-generation NOAA GFDL Atmospheric Model, version 4 (AM4) to simulate observed wintertime fine particulate matter (PM2.5) and its relationship to meteorology over Northern India. We compare two simulations of GFDL-AM4 nudged to observed meteorology for the period 1980–2016 driven by pollutant emissions from two global inventories developed in support of the Coupled Model Intercomparison Project Phases 5 (CMIP5) and 6 (CMIP6), and compare results with ground-based observations from India’s Central Pollution Control Board (CPCB) for the period 1 October 2015–31 March 2016. Overall, our results indicate that the simulation with CMIP6 emissions produces improved concentrations of pollutants over the region relative to the CMIP5-driven simulation. While the particulate concentrations simulated by AM4 are biased low overall, the model generally simulates the magnitude and daily variability of observed total PM2.5. Nitrate and organic matter are the primary components of PM2.5 over Northern India in the model. On the basis of correlations of the individual model components with total observed PM2.5 and correlations between the two simulations, meteorology is the primary driver of daily variability. The model correctly reproduces the shape and magnitude of the seasonal cycle of PM2.5, but the simulated diurnal cycle misses the early evening rise and secondary maximum found in the observations. Observed PM2.5 abundances are by far the highest within the densely populated IndoGangetic Plain, where they are closely related to boundary layer meteorology, specifically relative humidity, wind speed, boundary layer height, and inversion strength. The GFDL AM4 model reproduces the overall observed pollution gradient over Northern India as well as the strength of the meteorology–PM2.5 relationship in most locations.