the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Composition and sources of carbonaceous aerosol in the European Arctic at Zeppelin Observatory, Svalbard
Abstract. Our current understanding of Arctic carbonaceous aerosol (CA) is rudimentary and there is a lack of long-term observations for many components, such as organic aerosol (OA), exceptions to this include equivalent black carbon (eBC) and methane sulfonic acid (MSA).
To address this, we analyzed long-term measurements of organic carbon (OC), elemental carbon (EC), and source-specific organic tracers from 2017 to 2020 to constrain CA sources in the rapidly changing Arctic. We also used absorption photometer (aethalometer) measurements to constrain equivalent BC from biomass burning (eBCBB) and fossil fuel combustion (eBCFF) using Positive Matrix Factorization (PMF).
Our analysis showed that organic tracers are essential to understand Arctic CA sources. For 2017 to 2020, levoglucosan had a bimodal seasonality, with a signal from residential wood combustion (RWC) in the heating season (H-season; November to May) and from wildfires (WF) in the non-heating season (NH-season; June to October), demonstrating a pronounced inter-annual variability in the WF influence. Biogenic secondary organic aerosol (BSOA) species (2-methyltetrols) from isoprene oxidation appeared only in the NH-season, peaking in July to August. Intrusions of warm air masses from Siberia in summer caused three- and ninefold increases in 2-methyltetrols compared to 2017 to 2018, in 2019 and 2020, respectively, warranting investigation of the local vs. the long-range atmospheric transport (LRT) contribution, as certain Arctic vegetation has highly temperature sensitive biogenic volatile organic compounds (BVOC) emission rates. Primary biological aerosol particles (PBAP) tracers (various sugars and sugar-alcohols) were elevated in the NH-season but evolved differently, whereas cellulose was completely decoupled from the other PBAP tracers. Peak levels of most PBAP tracers and of 2-methyltetrols were associated with WF emissions, demonstrating the importance of measuring a broad spectrum of source specific tracers to understand sources and dynamics of CA. Finally, CA seasonality is heavily influenced by long-range atmospheric transport (LRT) episodes, since background levels are extremely low. E.g., we find the OA peak in the NH-season is as strongly influenced by LRT as is EC during Arctic Haze (AH).
Source apportionment of CA by Latin Hypercube Sampling (LHS) showed a mixed contribution from RWC (46 %), fossil fuel (FF) sources (27 %), and BSOA (25 %) in the H-season, whereas BSOA (56 %) prevailed over WF (26 %) and FF (15 %) in the NH-season. Source apportionment of eBC by PMF showed that FF combustion dominated eBC (70 ± 2.7 %), whereas RWC (22 ± 2.7 %) was more abundant than WF (8.0 ± 2.9 %). Modeled BC concentrations from FLEXPART attributed an almost equal share to FF (51 ± 3.1 %) and BB. Both FLEXPART and the PMF analysis concluded that RWC is a more important source than WF. However, with a modeled RWC of 30 ± 4.1 % and WF of 19 ± 2.8 %, FLEXPART suggests relatively higher contributions to eBC from these sources.
We find that OA (281 ± 106 ng m−3) is a significant fraction of the Arctic PM10 aerosol particle mass, though less than sea salt aerosol (SSA) (682 ± 46.9 ng m−3) and mineral dust (MD) (613 ± 368 ng m−3) as well as typically non-sea-salt sulfate (nssSO42−) (314 ± 62.6 ng m−3), originating mainly from anthropogenic sources in winter and from natural sources in summer. FF combustion was the prevailing source of eBC, whereas RWC made a larger contribution to eBCBB than WF.
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Notice on discussion status
The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
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The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
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Journal article(s) based on this preprint
Interactive discussion
Status: closed
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RC1: 'Comment on egusphere-2023-615', Anonymous Referee #1, 05 Jun 2023
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-615/egusphere-2023-615-RC1-supplement.pdf
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AC1: 'Reply on RC1', Karl Espen Yttri, 15 Nov 2023
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-615/egusphere-2023-615-AC1-supplement.pdf
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AC1: 'Reply on RC1', Karl Espen Yttri, 15 Nov 2023
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RC2: 'Comment on egusphere-2023-615', Anonymous Referee #2, 15 Jun 2023
The manuscript by Yttri et al. presents four years of observations of carbonaceous aerosols at an arctic site. The sources are investigated through measurements of specific organic source tracers combined with source apportionment and compared with dispersion modeling (FLEXPART).
Overall the study is interesting and important, and my comments are generally to the presentation of the study.
A very large number of abbreviations are used in the manuscript of which many are introduced already in the introduction. I suggest to reduce the number of abbreviations as it makes the manuscript difficult to read. Please also check that:
1. all abbreviations are only introduced once (e.g. LRT is explained twice in the abstract).
2. all abbreviations are actually used later in the text. If not, they are not necessary and just add to difficulty of reading the manuscript.Line 116-152: These paragraphs argue about the importance of the present work, but the authors have chosen a somewhat critical tone towards previous studies to highlight the importance of the present work. The readers will appreciate this work without the negative tone towards previous studies. I suggest to revise accordingly.
I suggest to add more information to introduce the source specific tracers in the introduction. This will be helpful for the readers to understand the results and discussion about e.g. ratios of levoglucosan and mannosan.
L440-449: Can local influence be completely excluded, in particular for RWC?
In general, it is useful to include standard deviations with average concentrations and contributions e.g. line 568-569.
Minor comments
Line 43-45: This introduction is confusing – “lack of long-term observations for many components such as OA” but then it is stated that the exception is eBC and MSA. I suggest to change “many” to “important” or similar.
L57-58 “compared to 2017 to 2018, in 2019 and 2020” – please clarify.
L73-74 more important source to eBC?
L86: Please add references to all statements.
L95-96: It is not clear to me how the Ng and McFiggans papers support this statement. Please clarify in your response.
L96: These changes may? Otherwise a reference is needed.
L148: tricarboxylic acid (please add a space before acid)
L149: Hansen et al. ACP 2014 (already a reference) reported monoterpene oxidation products in aerosols collected at two Arctic sites during a full year.
L224: Please add information about where standards were obtained.
L355-358: Please include the numbers here to make the comparison more clear. Were the Antarctica measurements part of the present study?
L363: Time series of EC, OC and sulfate?
L377: more efficient transport of polluted air masses?
L393: greatly. I suggest to change to considerably or significantly
L415-427: Please also explain the significance of the levoglucosan to mannosan ratio.
L439-440: Of EC?
L522: isoprene is the BVOC emitted in highest amount, not the most abundant.
L533: Please direct the reader to these data.
L580-584: I suggest to divide into two sentences.
L588-592: This part seems to need additional editing. The dashes seem to indicate that this is from a draft version.
L631: Larger contribution to PBAP in the Arctic?
L641: Where can the reader see this data?
L740: I suggest to include a more recent reference such as Glasius et al., Atmospheric Environment, 173, 127-141 (2018)
L793- : Please provide brief information about what was discussed in Zwaaftink et al. compared to the current study.Citation: https://doi.org/10.5194/egusphere-2023-615-RC2 -
AC2: 'Reply on RC2', Karl Espen Yttri, 15 Nov 2023
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-615/egusphere-2023-615-AC2-supplement.pdf
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AC2: 'Reply on RC2', Karl Espen Yttri, 15 Nov 2023
Interactive discussion
Status: closed
-
RC1: 'Comment on egusphere-2023-615', Anonymous Referee #1, 05 Jun 2023
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-615/egusphere-2023-615-RC1-supplement.pdf
-
AC1: 'Reply on RC1', Karl Espen Yttri, 15 Nov 2023
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-615/egusphere-2023-615-AC1-supplement.pdf
-
AC1: 'Reply on RC1', Karl Espen Yttri, 15 Nov 2023
-
RC2: 'Comment on egusphere-2023-615', Anonymous Referee #2, 15 Jun 2023
The manuscript by Yttri et al. presents four years of observations of carbonaceous aerosols at an arctic site. The sources are investigated through measurements of specific organic source tracers combined with source apportionment and compared with dispersion modeling (FLEXPART).
Overall the study is interesting and important, and my comments are generally to the presentation of the study.
A very large number of abbreviations are used in the manuscript of which many are introduced already in the introduction. I suggest to reduce the number of abbreviations as it makes the manuscript difficult to read. Please also check that:
1. all abbreviations are only introduced once (e.g. LRT is explained twice in the abstract).
2. all abbreviations are actually used later in the text. If not, they are not necessary and just add to difficulty of reading the manuscript.Line 116-152: These paragraphs argue about the importance of the present work, but the authors have chosen a somewhat critical tone towards previous studies to highlight the importance of the present work. The readers will appreciate this work without the negative tone towards previous studies. I suggest to revise accordingly.
I suggest to add more information to introduce the source specific tracers in the introduction. This will be helpful for the readers to understand the results and discussion about e.g. ratios of levoglucosan and mannosan.
L440-449: Can local influence be completely excluded, in particular for RWC?
In general, it is useful to include standard deviations with average concentrations and contributions e.g. line 568-569.
Minor comments
Line 43-45: This introduction is confusing – “lack of long-term observations for many components such as OA” but then it is stated that the exception is eBC and MSA. I suggest to change “many” to “important” or similar.
L57-58 “compared to 2017 to 2018, in 2019 and 2020” – please clarify.
L73-74 more important source to eBC?
L86: Please add references to all statements.
L95-96: It is not clear to me how the Ng and McFiggans papers support this statement. Please clarify in your response.
L96: These changes may? Otherwise a reference is needed.
L148: tricarboxylic acid (please add a space before acid)
L149: Hansen et al. ACP 2014 (already a reference) reported monoterpene oxidation products in aerosols collected at two Arctic sites during a full year.
L224: Please add information about where standards were obtained.
L355-358: Please include the numbers here to make the comparison more clear. Were the Antarctica measurements part of the present study?
L363: Time series of EC, OC and sulfate?
L377: more efficient transport of polluted air masses?
L393: greatly. I suggest to change to considerably or significantly
L415-427: Please also explain the significance of the levoglucosan to mannosan ratio.
L439-440: Of EC?
L522: isoprene is the BVOC emitted in highest amount, not the most abundant.
L533: Please direct the reader to these data.
L580-584: I suggest to divide into two sentences.
L588-592: This part seems to need additional editing. The dashes seem to indicate that this is from a draft version.
L631: Larger contribution to PBAP in the Arctic?
L641: Where can the reader see this data?
L740: I suggest to include a more recent reference such as Glasius et al., Atmospheric Environment, 173, 127-141 (2018)
L793- : Please provide brief information about what was discussed in Zwaaftink et al. compared to the current study.Citation: https://doi.org/10.5194/egusphere-2023-615-RC2 -
AC2: 'Reply on RC2', Karl Espen Yttri, 15 Nov 2023
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-615/egusphere-2023-615-AC2-supplement.pdf
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AC2: 'Reply on RC2', Karl Espen Yttri, 15 Nov 2023
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The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
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