| 1. |
- Bosch, Carme, et al.
(författare)
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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
- 2014
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Ingår i: Journal of Geophysical Research - Atmospheres. - 2169-897X .- 2169-8996. ; 119:20, s. 11743-11759
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 2. |
- Budhavant, Krishnakant, et al.
(författare)
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Anthropogenic fine aerosols dominate the wintertime regime over the northern Indian Ocean
- 2018
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Ingår i: Tellus. Series B, Chemical and physical meteorology. - : Stockholm University Press. - 0280-6509 .- 1600-0889. ; 70
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Tidskriftsartikel (refereegranskat)abstract
- This study presents and evaluates the most comprehensive set to date of chemical, physical and optical properties of aerosols in the outflow from South Asia covering a full winter (Nov. 2014 - March 2015), here intercepted at the Indian Ocean receptor site of the Maldives Climate Observatory in Hanimaadhoo (MCOH). Cluster analysis of air-mass back trajectories for MCOH, combined with AOD and meteorological data, demonstrate that the wintertime northern Indian Ocean is strongly influenced by aerosols transported from source regions with three major wind regimes, originating from the Indo-Gangetic Plain (IGP), the Bay of Bengal (BoB) and the Arabian Sea (AS). As much as 97 +/- 3% of elemental carbon (EC) in the PM10 was also found in the fine mode (PM2.5). Other mainly anthropogenic constituents such as organic carbon (OC), non-sea-salt (nss) -K+, nss-SO42- and NH4+ were also predominantly in the fine mode (70-95%), particularly in the air masses from IGP. The combination at this large-footprint receptor observatory of consistently low OC/EC ratio (2.0 +/- 0.5), strong linear relationships between EC and OC as well as between nss-K+ and both OC and EC, suggest a predominance of primary sources, with a large biomass burning contribution. The particle number-size distributions for the air masses from IGP and BoB exhibited clear bimodal shapes within the fine fraction with distinct accumulation (0.1m0.03. Taken together, the aerosol pollution over the northern Indian Ocean in the dry season is dominated by a well-mixed long-range transported regime of the fine-mode aerosols largely from primary combustion origin.
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| 3. |
- Budhavant, Krishnakant, et al.
(författare)
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Apportioned contributions of PM2.5 fine aerosol particles over the Maldives (northern Indian Ocean) from local sources vs long-range transport
- 2015
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Ingår i: Science of the Total Environment. - : Elsevier BV. - 0048-9697 .- 1879-1026. ; 536, s. 72-78
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Tidskriftsartikel (refereegranskat)abstract
- 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 main-land South Asia, there are also local Maldivian emissions. The local contributions to the load of fine particulate matter (PM2.5) in the Maldivian capital Male 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 Male 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 Male are higher (avg. 19 mu g/m(3)) than at MCOH (avg. 13 mu g/m(3)) with the difference being the largest during the summer, when local emissions play a larger role. The 24-hWorld Health Organization (WHO) PM2.5 health guideline was surpassed for the week-long collections in 71% of the cases in Male and in 74% of the cases for Hanimaadhoo. This study shows that in the dry/winter season 90 +/- 11% of PM2.5 levels in Male 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 Male and 13% at MCOH, suggesting larger contributions from incomplete combustion practices in the Male local region.
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| 4. |
- Budhavant, Krishnakant, et al.
(författare)
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Black carbon aerosols over Indian Ocean have unique source fingerprint and optical characteristics during monsoon season
- 2023
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Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : Proceedings of the National Academy of Sciences. - 0027-8424 .- 1091-6490. ; 120:8
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Tidskriftsartikel (refereegranskat)abstract
- Effects of aerosols such as black carbon (BC) on climate and buildup of the monsoon over the Indian Ocean are insufficiently quantified. Uncertain contributions from various natural and anthropogenic sources impede our understanding. Here, we use observations over 5 y of BC and its isotopes at a remote island observatory in northern Indian Ocean to constrain loadings and sources during little-studied monsoon season. Carbon-14 data show a highly variable yet largely fossil (65 ± 15%) source mixture. Combining carbon-14 with carbon-13 reveals the impact of African savanna burning, which occasionally approach 50% (48 ± 9%) of the total BC loadings. The BC mass-absorption cross-section for this regime is 7.6 ± 2.6 m2/g, with higher values during savanna fire input. Taken together, the combustion sources, longevity, and optical properties of BC aerosols over summertime Indian Ocean are different than the more-studied winter aerosol, with implications for chemical transport and climate model simulations of the Indian monsoon.
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| 5. |
- Budhavant, Krishnakant, et al.
(författare)
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Enhanced Light-Absorption of Black Carbon in Rainwater Compared With Aerosols Over the Northern Indian Ocean
- 2020
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Ingår i: Journal of Geophysical Research - Atmospheres. - 2169-897X .- 2169-8996. ; 125:2
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Tidskriftsartikel (refereegranskat)abstract
- Black carbon (BC) aerosols affect climate, especially in high aerosol loading regions such as South Asia. A key uncertainty for the climate effects of BC is the evolution of light-absorbing properties in the atmosphere. Here, we present a year-round comparison of the mass absorption cross section (MAC; 678 nm) of BC in air (PM10) and rain, for samples collected at the Maldives Climate Observatory at Hanimaadhoo. We develop a filter-loading correction scheme for estimating BC absorption on filters used in high-volume samplers. The year-round average MAC(678) of BC in the rain is almost twice (13.3 +/- 4.2 m(2)/g) compared to the PM10 aerosol (7.2 +/- 2.6 m(2)/g). A possible explanation is the elevated ratio of organic carbon (OC) to BC observed in rain particulate matter (9.4 +/- 6.3) compared to in the aerosols (OC/BC 2.6 +/- 1.4 and water-insoluble organic carbon/BC 1.2 +/- 0.8), indicating a coating-enhancement effect. In addition to BC, we also investigated the MAC(365) of water-soluble brown carbon in PM10 (0.4 +/- 0.4 m(2)/g, at 365 nm). In contrast to BC, MAC(365)brown carbon relates to air mass history, showing higher values for samples from air originating over the South Asian landmass. Furthermore, calculated washout ratios are much lower for BC compared to OC and inorganic ions such as sulfate, implying a longer atmospheric lifetime for BC. The wet deposition flux for BC during the high loading winter was 3 times higher than during the wet summer, despite much less precipitation in the winter.
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| 6. |
- Budhavant, Krishnakant, et al.
(författare)
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Radiocarbon-based source apportionment of elemental carbon aerosols at two South Asian receptor observatories over a full annual cycle
- 2015
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Ingår i: Environmental Research Letters. - : IOP Publishing. - 1748-9326. ; 10:6
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Tidskriftsartikel (refereegranskat)abstract
- 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 C-14-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 (f(bio)) was 53 +/- 5% (n = 6) atMCOHand 56 +/- 3% at SINH (n = 5). The f(bio) for the non-winter remainder was 53 +/- 11% (n = 6) atMCOHand 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 (f(bio)) EI spanning 55-88%, suggesting that most current EI for Indian BC systematically under predict the relative contribution of fossil fuel combustion. Acontinued 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.
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| 7. |
- Chandrika Ranjendra Nair, Hari Ram, 1989-, et al.
(författare)
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Aerosol demasking enhances climate warming over South Asia
- 2023
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Ingår i: npj Climate and Atmospheric Science. - 2397-3722. ; 6
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Tidskriftsartikel (refereegranskat)abstract
- Anthropogenic aerosols mask the climate warming caused by greenhouse gases (GHGs). In the absence of observational constraints, large uncertainties plague the estimates of this masking effect. Here we used the abrupt reduction in anthropogenic emissions observed during the COVID-19 societal slow-down to characterize the aerosol masking effect over South Asia. During this period, the aerosol loading decreased substantially and our observations reveal that the magnitude of this aerosol demasking corresponds to nearly three-fourths of the CO2-induced radiative forcing over South Asia. Concurrent measurements over the northern Indian Ocean unveiled a ~7% increase in the earth’s surface-reaching solar radiation (surface brightening). Aerosol-induced atmospheric solar heating decreased by ~0.4 K d−1. Our results reveal that under clear sky conditions, anthropogenic emissions over South Asia lead to nearly 1.4 W m−2 heating at the top of the atmosphere during the period March–May. A complete phase-out of today’s fossil fuel combustion to zero-emission renewables would result in rapid aerosol demasking, while the GHGs linger on.
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| 8. |
- Chandrika Ranjendra Nair, Hari Ram, 1989-, et al.
(författare)
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Aerosol demasking enhances climate warming over South Asia
- 2023
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Ingår i: npj Climate and Atmospheric Science. - 2397-3722. ; 6:1
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Tidskriftsartikel (refereegranskat)abstract
- Anthropogenic aerosols mask the climate warming caused by greenhouse gases (GHGs). In the absence of observational constraints, large uncertainties plague the estimates of this masking effect. Here we used the abrupt reduction in anthropogenic emissions observed during the COVID-19 societal slow-down to characterize the aerosol masking effect over South Asia. During this period, the aerosol loading decreased substantially and our observations reveal that the magnitude of this aerosol demasking corresponds to nearly three-fourths of the CO2-induced radiative forcing over South Asia. Concurrent measurements over the northern Indian Ocean unveiled a ~7% increase in the earth’s surface-reaching solar radiation (surface brightening). Aerosol-induced atmospheric solar heating decreased by ~0.4 K d−1. Our results reveal that under clear sky conditions, anthropogenic emissions over South Asia lead to nearly 1.4 W m−2 heating at the top of the atmosphere during the period March–May. A complete phase-out of today’s fossil fuel combustion to zero-emission renewables would result in rapid aerosol demasking, while the GHGs linger on.
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| 9. |
- Dasari, Sanjeev, et al.
(författare)
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Observation-constrained atmospheric lifetime and emission fluxes of black carbon aerosols over South Asia
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Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- Black carbon (BC) aerosols cause climate perturbation and affect air quality/human health. In densely populated South Asia—where the warming effect of BC is estimated to be ~ orders of magnitude higher than the global average—model simulations underestimate the wintertime atmospheric abundance of BC relative to surface observations. Two possible explanations for this model-observation offset are ill-constrained regional emission fluxes and atmospheric BC lifetime (τBC). Here, we combine hourly-resolved BC and carbon monoxide (CO) measurements for three successive winters from a South Asian receptor site—the Maldives Climate Observatory at Hanimaadhoo (MCOH)—in inverse frameworks, to assess the impact of emissions fluxes and lifetimes on ambient BC concentrations. The average ΔBC/ΔCO ratio (background corrected) at MCOH of 14±5 ng m-3 ppb-1 is found to be 2-3 times higher than in the East Asian outflow (range: 2 to 8 ng m-3 ppb-1). A BC transport efficiency of ~86% suggests low influence of wet scavenging processes during the dry South Asian winter period. Using statistical time series analysis, the τBC for dry wintertime South Asia is estimated to be 8±0.5 days, which is higher than commonly used in models. By coupling air mass back trajectories, lifetimes, and the ΔBC/ΔCO time-series data within an inverse modelling framework, we provide an observation-based “top-down” BC emission flux for South Asia estimated to be ~2.4±1 Tg/year. This is significantly higher than estimates from current “bottom-up” emission inventories (EIs). Taken together, this study suggests that to reconcile long-standing BC model-observation offsets in South Asia, existing emission estimates may need to be more than doubled in magnitude.
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| 10. |
- Dasari, Sanjeev, 1989-, et al.
(författare)
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Observational Evidence of Large Contribution from Primary Sources for Carbon Monoxide in the South Asian Outflow
- 2022
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 56:1, s. 165-174
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Tidskriftsartikel (refereegranskat)abstract
- South Asian air is among the most polluted in the world, causing premature death of millions and asserting a strong perturbation of the regional climate. A central component is carbon monoxide (CO), which is a key modulator of the oxidizing capacity of the atmosphere and a potent indirect greenhouse gas. While CO concentrations are declining elsewhere, South Asia exhibits an increasing trend for unresolved reasons. In this paper, we use dual-isotope (δ13C and δ18O) fingerprinting of CO intercepted in the South Asian outflow to constrain the relative contributions from primary and secondary CO sources. Results show that combustion-derived primary sources dominate the wintertime continental CO fingerprint (fprimary ∼ 79 ± 4%), significantly higher than the global estimate (fprimary ∼ 55 ± 5%). Satellite-based inventory estimates match isotope-constrained fprimary-CO, suggesting observational convergence in source characterization and a prospect for model–observation reconciliation. This “ground-truthing” emphasizes the pressing need to mitigate incomplete combustion activities for climate/air quality benefits in South Asia.
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