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Absorption enhancement of black carbon aerosols and the aerosol-induced masking effect on warming over South Asia
Stockholm University, Faculty of Science, Department of Environmental Science.ORCID iD: 0000-0002-8989-9483
2024 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis examines the effects of black carbon (BC) and other aerosols on the regional climate, focusing on their climate-relevant optical properties and implications for radiative effects. We focus on South Asia, home to one-third of the worldwide population. The abrupt societal changes during the COVID-19 pandemic led to an unprecedented reduction in anthropogenic emissions and provided a unique opportunity to study the impact of aerosol demasking on global warming. The thesis revolves around insights obtained from three atmospheric receptor observatories intercepting the outflow from South Asia, complemented by remote sensing data and aerosol modeling. These are:  Bangladesh Climate Observatory at Bhola (BCOB), positioned at the exit of the highly polluted Indo-Gangetic Plain (IGP), Maldives Climate Observatory at Hanimaadhoo (MCOH) in the Northern Indian Ocean, and Maldives Climate Observatory at Gan (MCOG) near the equator in the Indian Ocean. These observatories hence facilitate the measurements of aerosol properties from source regions to distant receptor environments and provide a comprehensive framework for assessing BC's regional climate impacts.

The thesis offers insights into the changes in the sources of BC and the resultant climatic impact. The thesis quantifies the changes in the regional aerosol properties resulting from reduced anthropogenic emissions during the COVID-19 pandemic societal shutdown. The study reveals a substantial decrease in atmospheric aerosol loading, resulting in a reduction of the aerosol forcing roughly three-fourths of the magnitude of CO2-induced radiative forcing at the top of the atmosphere and a ~7% increase in surface-reaching solar radiation. This work also demonstrates a notable shift in relative contribution of BC sources at BCOB during the COVID period: fossil fuel contributions decreased from 49% to 35%, while C3 biomass burning increased from 31% to 55%, with C4 biomass remaining a minor source. Similarly, for MCOH, reflecting the outflow from the greater South Asian subcontinent, the contribution from fossil combustion decreased while C3 combustion increased.

Further, the thesis explores the optical properties of BC, coating effects, and changes in mass absorption cross section (MAC) during long-range transport. The study shows a uniform MAC enhancement from water-soluble coatings of 1.6±0.5 across sites BCOB, MCOH and MCOG. However, the BC MAC increased by 80% in two separate studies from the IGP outflow at BCOB to the Indian Ocean receptor stations, suggesting a common underlying phenomenon.  This mechanism is likely linked to scavenging fractionation occurring during the long-range transport of BC, which selectively filters out larger, lower BC MAC particles. This results in a residual population of finer, hydrophobic BC particles characterized by a notably higher MAC678 at the receptor observatories in Northern Indian Ocean. Additionally, throughout the transport from the BCOB to the MCOH, BC particles undergo a transformation, becoming more absorbent—akin to becoming "darker." This transformation is facilitated by the photochemical bleaching of organic carbon (OC) and in-cloud processes, which further contribute to the increase in BC- BC-MAC678. On the other hand, BrC-MAC decreased due to photochemical bleaching.

The findings of this thesis, based on observations, enhance our understanding of the constantly changing optical and radiative impact of human-made aerosols in the highly significant South Asian emission region. This, in turn, enables better descriptions of the evolving aerosol characteristics in climate models and offers guidance for informed policy-making and the development of effective climate mitigation strategies.

Place, publisher, year, edition, pages
Stockholm: Department of Environmental Science, Stockholm University , 2024. , p. 49
Keywords [en]
Black Carbon, Climate Impact, Aerosol Transport, COVID-19 impact on Emissions
National Category
Climate Science Meteorology and Atmospheric Sciences
Research subject
Environmental Sciences
Identifiers
URN: urn:nbn:se:su:diva-228618ISBN: 978-91-8014-805-4 (print)ISBN: 978-91-8014-806-1 (electronic)OAI: oai:DiVA.org:su-228618DiVA, id: diva2:1853820
Public defence
2024-06-10, Högbomsalen, Geovetenskapens hus, Svante Arrhenius väg 14, Stockholm, 13:00 (English)
Supervisors
Available from: 2024-05-16 Created: 2024-04-23 Last updated: 2025-02-01Bibliographically approved
List of papers
1. Aerosol demasking enhances climate warming over South Asia
Open this publication in new window or tab >>Aerosol demasking enhances climate warming over South Asia
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2023 (English)In: npj Climate and Atmospheric Science, E-ISSN 2397-3722, Vol. 6, article id 39Article in journal (Refereed) Published
Abstract [en]

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.

National Category
Meteorology and Atmospheric Sciences Climate Science
Research subject
Atmospheric Sciences and Oceanography; Applied Environmental Science; Environmental Sciences
Identifiers
urn:nbn:se:su:diva-228565 (URN)10.1038/s41612-023-00367-6 (DOI)000991239400001 ()2-s2.0-85160091841 (Scopus ID)
Funder
The Royal Swedish Academy of Sciences, 2017−01601
Available from: 2024-04-22 Created: 2024-04-22 Last updated: 2025-02-01Bibliographically approved
2. Source apportionment of black carbon using radiocarbon and stable carbon isotopes during COVID-19 societal slowdown in South Asia
Open this publication in new window or tab >>Source apportionment of black carbon using radiocarbon and stable carbon isotopes during COVID-19 societal slowdown in South Asia
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

Black carbon (BC) aerosol emissions in South Asia perturb the regional climate system and significantly degrade the air quality, affecting the health and environment of approximately 1.5 billion people. This study investigates the alterations in BC sources during the societal slowdown during the 2020 COVID-19 pandemic, capitalizing on aerosol samples of the intercepted South Asian outflow at receptor stations of the Maldives Climate Observatory at Hanimaadhoo (MCOH) and the Bangladesh Climate Observatory at Bhola (BCOB). The study used dual-carbon isotopes (Δ14C and δ13C) to understand the impact of societal disruptions on BC levels and sources. The isotope source fingerprinting of BC in the outflow from the Indo-Gangetic Plain (at BCOB) revealed that for the COVID period, a decreasing contribution from fossil fuel (from 49% down to 35%) amidst an increase in the fraction from C3 biomass burning going from 31% to 55% with C4 biomass burning remaining as a minor contributor. Similarly, for MCOH, reflecting the outflow from the greater S Asian subcontinent, the contribution from fossil combustion decreased while C3 combustion correspondingly increased. This likely reflects both decreased transport and an increase in crop residue burning and the use of biomass for heating and cooking. These dual-isotope constraints demonstrate that a decisive shift in emissions of climate-forcing BC aerosols occurred during the pandemic slowdown, suggesting that a societal transformation away from fossil fuel reliance will quickly propagate into the aerosol composition over South Asia. 

Keywords
Air pollution, Aerosol chemical composition, Biomass burning, Pandemic, South Asia
National Category
Climate Science Meteorology and Atmospheric Sciences Environmental Sciences
Identifiers
urn:nbn:se:su:diva-228623 (URN)
Available from: 2024-04-23 Created: 2024-04-23 Last updated: 2025-02-01
3. Roles of water-soluble aerosol coatings for the enhanced radiative absorption of black carbon over south asia and the northern indian ocean
Open this publication in new window or tab >>Roles of water-soluble aerosol coatings for the enhanced radiative absorption of black carbon over south asia and the northern indian ocean
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2024 (English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 926, article id 171721Article in journal (Refereed) Published
Abstract [en]

Black Carbon (BC), formed by incomplete combustion, absorbs solar radiation and heats the atmosphere. We investigated the enhancement in optical absorption of BC due to coatings of water-soluble (WS) species in the polluted South Asian atmosphere. The BC Mass Absorption Cross-section (MAC; 678 nm) was estimated before and after removal of the WS components. Wintertime samples were collected from three South Asian receptor observatories intercepting large-footprint outflow: Bangladesh Climate Observatory Bhola (BCOB; integrating outflow of the Indo-Gangetic Plain), Maldives Climate Observatories at Hanimaadhoo (MCOH) and at Gan (MCOG), both reflecting outflow from the South Asian region. The ambient MAC observed at BCOB, MCOH and MCOG were 4.2 ± 1.4, 7.9 ± 1.9 and 7.1 ± 1.5 m2 g−1, respectively.

The average enhancement of the BC MAC due to WS coatings (i.e., ws-EMAC) was identical at all three sites (1.6 ± 0.5) indicating that the anthropogenic aerosols had already evolved to a fully coated morphology at BCOB and/or that subsequent aging involved two compensating evolution processes of the coating. Inspecting the key coating component sulfate; the sulfate-to-BC ratio increased threefold when transitioning from BCOB to MCOH and by about 1.5 times from BCOB to MCOG. Conversely, both WS organic carbon (WSOC)/BC and water-insoluble OC (WIOC)/BC ratios declined with distance: WSOC/BC diminished by 84 % from BCOB to MCOH and by 80 % from BCOB to MCOG, while WIOC/BC dropped by about 63 % and 59 %, respectively. Such declines in WSOC and WIOC reflect a combination of photochemical oxidation and more efficient washout of OC compared to BC. The observed changes in the SO42−/BC and WSOC/BC ratios across South Asia highlight the significant impact of aerosol composition on the optical properties of Black Carbon (BC). These findings emphasize the need for detailed studies on aerosol composition to improve climate models and develop effective strategies for reducing the impact of anthropogenic aerosols on the climate.

Keywords
Black carbon, Atmospheric Aerosols, Climate warming, Absorption Enhancement, Mass Absorption Enhancement, Water Soluble Organic Carbon
National Category
Meteorology and Atmospheric Sciences Climate Science Environmental Sciences
Identifiers
urn:nbn:se:su:diva-228619 (URN)10.1016/j.scitotenv.2024.171721 (DOI)001225020600001 ()38494028 (PubMedID)2-s2.0-85189032601 (Scopus ID)
Funder
Swedish Research Council
Available from: 2024-04-23 Created: 2024-04-23 Last updated: 2025-02-01Bibliographically approved
4. Changing optical properties of Black Carbon and Brown Carbon aerosols during long-range transport from the Indo-Gangetic Plain to the equatorial Indian Ocean
Open this publication in new window or tab >>Changing optical properties of Black Carbon and Brown Carbon aerosols during long-range transport from the Indo-Gangetic Plain to the equatorial Indian Ocean
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

Atmospheric aerosols strongly influence the global climate by their light absorption (e.g., black carbon, BC, brown carbon, BrC) and scattering (e.g., sulfate) properties. This study presents simultaneous measurements of ambient aerosol light absorption properties and chemical composition from three large-footprint South Asian receptor sites during the South Asian Pollution Experiment (SAPOEX) in December 2017 - March 2018. The BC mass absorption cross-section (BC-MAC678) values increased from 3.5 ± 1.3 at the Bhola Climate Observatory-Bangladesh (i.e., located at exit outflow of Indo-Gangetic Plain) to 6.4 ± 1.3 at the two regional receptor observatories at Maldives Climate Observatory-Hanimaadhoo (MCOH) and Maldives Climate Observatory-Gan (MCOG), an increase of 80%. This likely reflects a scavenging fractionation resulting in a population of finer BC with higher MAC678 having higher longevity. At the same time, the BrC-MAC365 decreased by a factor of three from the IGP exit to the equatorial Indian Ocean, likely due to photochemical bleaching of organic chromophores. The high chlorine-to-sodium ratio at the near-source-region BCOB suggests a significant contribution of chlorine from anthropogenic activities. This particulate Cl- has the potential to convert into Cl-radicals that can affect the oxidation capacity of the polluted air. Moreover, Cl- is shown to be near-fully consumed during the long-range transport. The results of this synoptic study over the large South Asian scale contribute rare observational constraints on optical properties of ambient BC (and BrC) aerosols over regional scales away from emission sources. It also contributes significantly to understanding the ageing effect of the optical and chemical properties of aerosols as the pollution from the Indo-Gangetic Plain disperses over the tropical ocean.

National Category
Meteorology and Atmospheric Sciences Climate Science Environmental Sciences
Identifiers
urn:nbn:se:su:diva-228620 (URN)
Available from: 2024-04-23 Created: 2024-04-23 Last updated: 2025-02-01

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