Krishnakant Budhavant

Source-diagnostic dual-isotope composition and optical properties of water-soluble organic carbon and elemental carbon in the South Asian outflow intercepted over the Indian Ocean

The dual carbon isotope signatures and optical properties of carbonaceous aerosols have been investigated simultaneously for the first time in the South Asian outflow during an intensive campaign at the Maldives Climate Observatory on Hanimaadhoo (MCOH) (February and March 2012). As one component of the Cloud Aerosol Radiative Forcing Dynamics Experiment, this paper reports on the sources and the atmospheric processing of elemental carbon (EC) and water-soluble organic carbon (WSOC) as examined by a dual carbon isotope approach. The radiocarbon (C-14) data show that WSOC has a significantly higher biomass/biogenic contribution (865%) compared to EC (594%). The more C-13-enriched signature of MCOH-WSOC (-20.80.7) compared to MCOH-EC (-25.8 +/- 0.3 parts per thousand) and megacity Delhi WSOC (-24.1 +/- 0.9 parts per thousand) suggests that WSOC is significantly more affected by aging during long-range transport than EC. The C-13-C-14 signal suggests that the wintertime WSOC intercepted over the Indian Ocean largely represents aged primary biomass burning aerosols. Since light-absorbing organic carbon aerosols (Brown Carbon (BrC)) have recently been identified as potential contributors to positive radiative forcing, optical properties of WSOC were also investigated. The mass absorption cross section of WSOC (MAC(365)) was 0.5 +/- 0.2 m(2)g(-1) which is lower than what has been observed at near-source sites, indicating a net decrease of WSOC light-absorption character during long-range transport. Near-surface WSOC at MCOH accounted for similar to 1% of the total direct solar absorbance relative to EC, which is lower than the BrC absorption inferred from solar spectral observations of ambient aerosols, suggesting that a significant portion of BrC might be included in the water-insoluble portion of organic aerosols.

Radiocarbon-based source apportionment of elemental carbon aerosols at two South Asian receptor observatories over a full annual cycle

Black carbon (BC) aerosols impact climate and air quality. Since BC from fossil versus biomass combustion have different optical properties and different abilities to penetrate the lungs, it is important to better understand their relative contributions in strongly affected regions such as South Asia. This study reports the first year-round 14C-based source apportionment of elemental carbon (EC), the mass-based correspondent to BC, using as regional receptor sites the international Maldives Climate Observatory in Hanimaadhoo (MCOH) and the mountaintop observatory of the Indian Institute of Tropical Meteorology in Sinhagad, India (SINH). For the highly-polluted winter season (December–March), the fractional contribution to EC from biomass burning (fbio) was 53 ± 5% (n = 6) at MCOH and 56 ± 3% at SINH (n = 5). The fbio for the non-winter remainder was 53 ± 11% (n = 6) at MCOH and 48 ± 8% (n = 7) at SINH. This observation-based constraint on near-equal contributions from biomass burning and fossil fuel combustion at both sites compare with predictions from eight technology-based emission inventory (EI) models for India of (fbio)EI spanning 55–88%, suggesting that most current EI for Indian BC systematically under predict the relative contribution of fossil fuel combustion. A continued iterative testing of bottom-up EI with top-down observational source constraints has the potential to lead to reduced uncertainties regarding EC sources and emissions to the benefit of both models of climate and air quality as well as guide efficient policies to mitigate emissions.

Seasonal factors influencing in chemical composition of total suspended particles at Pune, India.

A study on the chemical characterization of boundary layer aerosols is made based on the collection of TSP and size separated aerosol mass samples at Pune during March 2007-February 2008. This study will be helpful in simulating atmospheric processes responsible for aerosol development over Pune region and understanding its environmental implications related to radiation budget and climate. It is found that major fraction of Ca(2+) is locally generated by suspension of soil dust during all the seasons. During pre-monsoon season, coarse Mg(2+) is originated from the soil and the sea salt, whereas fine Mg(2+) is generated from the local biomass burning. Sizeable amount of SO(4)(2-) is emitted from local industrial and brick kilns activities. Neutralization of NO(3)(-), generated both from biogenic and anthropogenic sources, is made by NH(3) gas generated mainly from anthropogenic sources. The data are further examined in terms of the factors specific to the individual seasons influencing physical and chemical characteristics of the boundary layer aerosols. The specific factors are: (a) Intense local convection during pre-monsoon season; (b) southwesterly wind flow and rainfall activity during monsoon season; and (c) Day time convection and occurrence of low level inversion during post-monsoon and winter seasons.

Apportioned contributions of PM2.5 fine aerosol particles over the Maldives (northern Indian Ocean) from local sources vs long-range transport.

Urban-like plumes of gases and particulate matter originating from the South Asian region are frequently observed over the Indian Ocean, especially during the dry winter period. However, in addition to the strong sources on mainland South Asia, there are also local Maldivian emissions. The local contributions to the load of fine particulate matter (PM2.5) in the Maldivian capital Malé was assessed using the well-established Maldives Climate Observatory at Hanimaadhoo (MCOH) to represent local background, recording the long-range transported component for a full-year synoptic campaign at both sites in 2013. The year-round levels in both Malé and MCOH are strongly influenced by the seasonality of the monsoon cycle, including precipitation patterns and air-mass transport pathways, with lower levels during the wet summer season. The annual-average PM2.5 levels in Malé are higher (avg. 19 μg/m3) than at MCOH (avg. 13 μg/m3) with the difference being the largest during the summer, when local emissions play a larger role. The 24-h World Health Organization (WHO) PM2.5 health guideline was surpassed for the weeklong collections in 71% of the cases in Malé and in 74% of the cases for Hanimaadhoo. This study shows that in the dry/winter season 90±11% of PM2.5 levels in Malé could be from long-range transport with only 8±11% from local emissions while in the wet/monsoon season the relative contributions are about equal. The concentrations of organic carbon (OC) and elemental carbon (EC) showed similar seasonal patterns as bulk mass PM2.5. The relative contribution of total carbonaceous matter to bulk mass PM2.5 was 17% in Malé and 13% at MCOH, suggesting larger contributions from incomplete combustion practices in the Malé local region.

Wet Deposition of Nitrogen at Different Locations in India

The wet deposition data for Pune (2000–2007), for the other locations representing different environments (i.e., urban, rural, industrial, high altitude, marine, traffic etc.) for different time periods during 2001–2007, and for ten Global Atmospheric Watch (GAW) locations in India for a period of 8 years (2000–2007) are considered in this chapter. All the rain water samples were analyzed for pH, conductivity, anions (Cl, SO4 and NO3) and cations (NH4, Na, K, Ca and Mg). In general, in India the rain water was found to be in the alkaline range. Out of ten GAW stations, the 8 years average pH was slightly acidic (pH 5.15–5.36) at only three locations. At the remaining seven locations the pH was alkaline (pH > 5.65). This alkaline nature is due to high dust levels. Neutralization factors indicated that calcium (Ca) is the major neutralizing cation in wet deposition. Calcium concentrations were higher in north and northwestern regions and lower in southern and northeastern regions. Non-sea salt component and back trajectory analyses showed that Ca and SO4 aerosols were transported to the Indian sub-continent from North African and Gulf countries. The wet deposition fluxes were estimated for all the ionic components including nitrogen (N). The 8 year average annual wet deposition of N for ten locations varied between 4.7 and 34.3 kg N ha−1 year−1 and yearly depositions varied between 1.8 and 57 kg N ha−1 year−1. At all the locations, the NO3-N depositions were higher compared to NH4-N. At some of the locations, even though the concentrations are low, the depositions were higher due to the high rainfall amounts. In regional perspective, the excess SO4-S deposition was higher at an industrial location and the N deposition was higher at a traffic junction in Pune region. At a high altitude rural location (Sinhagad) nearby Pune, the concentrations of excess SO4, NO3 and NH4 were lower but their depositions were higher due to higher rainfall amounts. The total N deposition at four different locations in Pune region varied from 10.4 to 13.2 kg N ha−1 year−1.