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Lifecycle of Black Carbon in the Arctic
Stockholm University, Faculty of Science, Department of Environmental Science.ORCID iD: 0000-0003-1389-8713
2023 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This PhD thesis investigates the atmospheric life cycle of Black Carbon (BC) in the Arctic. The Arctic region has been rapidly changing in the last decades and the role of BC aerosols in this is still uncertain. BC aerosols are mainly produced by incomplete combustion of biomass burning and fossil fuel and stand out from other aerosol species due to their strong ability to absorb solar radiation. The impact of BC on the Earth’s radiation budget is estimated to be overall warming. While the indirect effect, interactions with clouds, is estimated to be negative, the direct radiation effect is positive because of the absorption ability of the BC. These estimates are uncertain, especially for aerosol-cloud interactions. To estimate the role of BC in the Arctic, it is necessary to know the size distribution of BC, the transport pattern and the loss processes that affect the BC concentration. In this thesis, in-situ observations from the Zeppelin observatory in the Arctic, as well as global modelling tools, are used to answer the following research questions: 1. What kind of new insights about BC size distributions can be gained from simultaneous long-term measurements of absorption and aerosol number size distributions? 2. How do source regions impact BC size distributions measured at Zeppelin? 3. How are observations of biomass burning tracers at Zeppelin connected to transport from source regions with active fires? 4. How do emissions, as well as, wet and dry removal pathways drive the diversity of the BC life cycle in General Circulation Models (GCMs)?

A statistical method to derive BC size distributions from filter-based absorption measurements was developed and applied to long-term data from the Arctic measurement station Zeppelin on Svalbard. Promising results were obtained for inferring BC number size distributions from absorption and size distribution data, except for the most polluted conditions with the air masses arriving from Northern Eurasia and Russia - as identified from an analysis using back trajectories. Trajectory analysis was also used to link events with elevated biomass burning tracers and BC at Zeppelin to fire activity measured by satellites on the continents around the Arctic. To investigate the interplay of emissions and removal processes of BC in models and to understand the diversity in model representation of BC in the Arctic, a detailed analysis of processes in four GCMs was performed. The BC concentrations in the Arctic were compared and their response to removal processes during long-range transport to Zeppelin. The results underline the importance of BC sources and processing far away from the Arctic.

The knowledge gained about the BC life cycle will facilitate a better assessment of the large-scale influence of BC on the Arctic climate and environment.

Place, publisher, year, edition, pages
Stockholm: Department of Environmental Science, Stockholm University , 2023. , p. 28
Keywords [en]
Black Carbon, Aerosols, Arctic, lifecyle, absorption
National Category
Environmental Sciences Meteorology and Atmospheric Sciences
Research subject
Environmental Sciences
Identifiers
URN: urn:nbn:se:su:diva-218085ISBN: 978-91-8014-396-7 (print)ISBN: 978-91-8014-397-4 (electronic)OAI: oai:DiVA.org:su-218085DiVA, id: diva2:1766835
Public defence
2023-10-18, De Geersalen, Geovetenskapens hus, Svante Arrhenius väg 14, Stockholm, 10:00 (English)
Opponent
Supervisors
Available from: 2023-09-11 Created: 2023-06-13 Last updated: 2025-02-01Bibliographically approved
List of papers
1. Airmass Analysis of Size-Resolved Black Carbon Particles Observed in the Arctic Based on Cluster Analysis
Open this publication in new window or tab >>Airmass Analysis of Size-Resolved Black Carbon Particles Observed in the Arctic Based on Cluster Analysis
2022 (English)In: Atmosphere, E-ISSN 2073-4433, Vol. 13, no 5, article id 648Article in journal (Refereed) Published
Abstract [en]

Here we apply new analysis methods and approaches to existing long-term measurement series that provide additional insights into the atmospheric processes that control black carbon (BC) in the Arctic. Based on clustering size distribution data from Zeppelin Observatory for the years 2002–2010, observations classified as ‘Polluted’ were further investigated based on BC properties. The data were split into two subgroups, and while the microphysical and chemical fingerprints of the two subgroups are very similar, they show larger differences in BC concentration and correlation with the particle size distribution. Therefore, a source–receptor analysis was performed with HYSPLIT 10-days backward trajectories for both subsets. We demonstrate that within this ‘Polluted’ category, the airmasses that contributed to the largest BC signal at the Zeppelin station are not necessarily associated with traditional transport pathways from Eurasia. Instead, the strongest signal is from a region east of the Ural Mountains across the continent to the Kamchatka Peninsula.

Keywords
carbonaceous aerosol, aerosol life cycle, light-absorbing particles, Svalbard, particle soot absorption photometer, absorption coefficient
National Category
Earth and Related Environmental Sciences
Identifiers
urn:nbn:se:su:diva-206877 (URN)10.3390/atmos13050648 (DOI)000803664500001 ()2-s2.0-85129424546 (Scopus ID)
Available from: 2022-06-30 Created: 2022-06-30 Last updated: 2025-02-07Bibliographically approved
2. Using correlations between observed equivalent black carbon and aerosol size distribution to derive size resolved BC mass concentration: a method applied on long-term observations performed at Zeppelin station, Ny-Ålesund, Svalbard
Open this publication in new window or tab >>Using correlations between observed equivalent black carbon and aerosol size distribution to derive size resolved BC mass concentration: a method applied on long-term observations performed at Zeppelin station, Ny-Ålesund, Svalbard
2021 (English)In: Tellus. Series B, Chemical and physical meteorology, ISSN 0280-6509, E-ISSN 1600-0889, Vol. 73, no 1, p. 1-17, article id 1933775Article in journal (Refereed) Published
Abstract [en]

The aim of this study was to explore particle size dependent properties by combining long-term observations of equivalent black carbon (eBC) and number size distributions to investigate their correlation as function of particle size. The work was conducted in two main parts. The first part consisted of a short laboratory experiment to compare observed total particle light absorption (σabs) with that observed according to particle size by using a combination of a Differential Mobility Analyzer (DMA) and a Particle Soot Absorption Photometer (PSAP). The laboratory study confirmed strong similarities between the observed and derived σabs. In the second part the statistical approach using correlation between the σabs and the dN of each bin of the number size distribution was tested on long-term data ranging from 2002 to 2010 observed at Zeppelin station, Ny-Ålesund Svalbard. The data was clustered according to the number size distribution and grouped in four major categories: Washout, Nucleation, Intermediate and Polluted. Each category presented different features with respect to the derived eBC mass distributions, the Intermediate category showed similarities to the few available Single Particle Soot Photometer (SP2) observations in the Arctic. Overall, the statistical distribution of eBC, according to particle size, presented a larger dynamical range in the location of the mode(s). To check for consistency, the eBC mass distributions were transformed into number based eBC size distribution and compared to the observed total number size distribution. Whereas the Washout, Nucleation and Intermediate categories presented plausible number distributions, the Polluted category displayed a mode at small sizes (about 50 nm) that was significantly exaggerated.

Keywords
carbonaceous aerosol, data mining, optical properties, cluster analysis, life cycle
National Category
Earth and Related Environmental Sciences
Identifiers
urn:nbn:se:su:diva-195735 (URN)10.1080/16000889.2021.1933775 (DOI)000661137100001 ()
Available from: 2021-08-25 Created: 2021-08-25 Last updated: 2025-02-07Bibliographically approved
3. Impact of biomass burning on Arctic aerosol composition
Open this publication in new window or tab >>Impact of biomass burning on Arctic aerosol composition
Show others...
(English)In: Article in journal (Other academic) Submitted
Keywords
Arctic aerosol, Zeppelin Observatory, FIGAERO-CIMS, aerosol chemical composition, biomass burning, agricultural fires
National Category
Earth and Related Environmental Sciences
Identifiers
urn:nbn:se:su:diva-219820 (URN)
Available from: 2023-08-02 Created: 2023-08-02 Last updated: 2025-02-07Bibliographically approved
4. Investigating the role of air mass history on the diversity of GCMestimates of atmospheric black carbon in the Arctic
Open this publication in new window or tab >>Investigating the role of air mass history on the diversity of GCMestimates of atmospheric black carbon in the Arctic
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

Black Carbon (BC) aerosols are known to play an important role in the Arctic, yet their exact contribution to thechanging of the Earth’s climate and Arctic amplification remains unclear. To reduce these uncertainties, the life cycle of BCneeds to be accurately described in general circulation models (GCMs). In this study, four GCMs (ECHAM6.3-HAM2.3,ECHAM6.3-HAM2.3-P3, ECHAM6.3-HAM2.3-SALSA2 and UKESM1.0) are compared in terms of their representation ofBC in the Arctic. A new Lagrangian framework is applied to investigate the history of airmasses reaching the Arctic observationalsite Zeppelin on Svalbard, and compared to the corresponding transport simulated by the GCMs, which are allnudged to reanalysis data from ERA-Interim. Aerosol processes along the trajectories are then compared between the models.ECHAM6.3-HAM2.3-P3 simulates the highest and UKESM1.0 the lowest BC loadings both globally and within the Arcticand ECHAM6.3-HAM2.3-SALSA2 is the GCM that reproduces the observations from Zeppelin station most faithfully. The BC concentration in the Arctic is largely controlled by the wet removal processes described in the models, but dry depositionalso plays a role in explaining some of the inter-model diversity. ECHAM6.3-HAM2.3-P3 is less efficient in wet removal thanthe other models, which is likely a result of an adjusted representation of ice processes compared with the other two ECHAMvariants. UKESM1.0 is the most efficient model in removing BC from the atmosphere, in large part due to more efficient dryremoval than with the ECHAM models. The Lagrangian analysis reveals that the BC concentrations at the Zeppelin station are largely determined by concentrations in airmasses older than the length of our back trajectories, i.e. ten days, highlighting theimportance of remote emissions to local BC concentrations in the Arctic. This further suggests a longer BC lifetime within theArctic as compared with the global average. Our results underline the importance of accurate descriptions of cloud and precipitation microphysics, along with realistic dry and wet scavenging schemes for improved descriptions of BC and its climateimpacts in the Arctic within GCMs.

Keywords
Black Carbon, Aerosols, Artic, scavenging, lifecyle, Aerocom
National Category
Natural Sciences Earth and Related Environmental Sciences Environmental Sciences
Research subject
Environmental Sciences; Atmospheric Sciences and Oceanography
Identifiers
urn:nbn:se:su:diva-220374 (URN)
Available from: 2023-08-25 Created: 2023-08-25 Last updated: 2025-01-31

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Cremer, Roxana S.

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