From the journal Environmental Science: Atmospheres Peer review history
Interference of sea salt in capture vaporizer-ToF-ACSM measurements of biomass burning organic aerosols in coastal locations
Round 1
Manuscript submitted on 08 dic. 2023![](https://www.rsc-cdn.org/pubs-core/2022.0.148/content/NewImages/icon-letter.png)
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15-Feb-2024
Dear Mr Sutresna:
Manuscript ID: EA-ART-12-2023-000171
TITLE: Interference of sea salt in capture vaporizer-ToF-ACSM measurements of biomass burning organic aerosols in coastal locations
Thank you for your submission to Environmental Science: Atmospheres, published by the Royal Society of Chemistry. I sent your manuscript to reviewers and I have now received their reports which are copied below.
I have carefully evaluated your manuscript and the reviewers’ reports, and the reports indicate that major revisions are necessary.
Please submit a revised manuscript which addresses all of the reviewers’ comments. Further peer review of your revised manuscript may be needed. When you submit your revised manuscript please include a point by point response to the reviewers’ comments and highlight the changes you have made. Full details of the files you need to submit are listed at the end of this email.
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Environmental Science: Atmospheres strongly encourages authors of research articles to include an ‘Author contributions’ section in their manuscript, for publication in the final article. This should appear immediately above the ‘Conflict of interest’ and ‘Acknowledgement’ sections. I strongly recommend you use CRediT (the Contributor Roles Taxonomy, https://credit.niso.org/) for standardised contribution descriptions. All authors should have agreed to their individual contributions ahead of submission and these should accurately reflect contributions to the work. Please refer to our general author guidelines https://www.rsc.org/journals-books-databases/author-and-reviewer-hub/authors-information/responsibilities/ for more information.
I look forward to receiving your revised manuscript.
Yours sincerely,
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Associate Editor, Environmental Science: Atmospheres
Environmental Science: Atmospheres is accompanied by companion journals Environmental Science: Nano, Environmental Science: Processes and Impacts, and Environmental Science: Water Research; publishing high-impact work across all aspects of environmental science and engineering. Find out more at: http://rsc.li/envsci
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Responses to reviewer comments:
We would like to thank the referees for their insightful comments and questions for this submitted paper.
We intend to use this space to address comments and questions raised by both referees given their significance to the content of the revised manuscript.
Comments regarding using PMF (major comment 1 from Referee 1, major comment 2 from Referee 2) to separate the influences of biomass burning and sea salt to m/z 60 were particularly appreciated. We applied this technique to the COALA dataset as well as part of the KCG dataset, which we found to yield factors that represented organic aerosols from both sea salt and biomass burning, with those factors containing m/z 60. As a result, we added Section 3.2 (“PMF”) which describes in detail the factors in each location that contain m/z 60. Here, we estimated the sources of these factors by analysing f60, the other prominent marker ions (illustrated in Section S5 in the Supplementary), and their correlations with biomass burning and sea salt markers. Inclusion of this PMF analysis in our paper has also necessitated changes to the text in Section 1 (“Introduction”), Section 2 (“Methods”), Section 4 (“Discussion”), and Section 5 (“Conclusion”).
Another change that has impacted multiple sections of the manuscript (on investigation in response to major comment 3, minor comment 4 raised by Referee 1; as well as minor comment 7 raised by Referee 2) is that references to the difference between f60/f73 ratios when using the different vaporizers have been removed from Sections 1, 3, 4, and 5. This was because the claim made regarding f60/f73 ratios being generally higher when using the standard vaporizer was found to be less conclusive upon further investigation of BBOA spectra found on the AMS spectral database (https://cires1.colorado.edu/jimenez-group/AMSsd_CV/). Despite this change, the original conclusions of the paper remain unchanged.
Section 6 (“Future Work”) has also been added to address some valid and constructive points that were raised but warrant further study in separate publications. These include:
• Evaluating marker ions that are more appropriate to use with the CV-ToF-ACSM (major comment 4 from Referee 1 and major comment 1 from Referee 2), including those proposed in Hu et al. (2018) – while important, we believe that this paper’s goal is to identify and characterise an issue with a marker ion that is currently in common use when identifying biomass burning organic aerosols (m/z 60).
• Investigating the mechanism of sea salt interference (major comment 6 from Referee 1) – we have mentioned the need to perform more detailed source apportionment regarding the contribution of multiple sources of m/z 60 using the capture vaporizer-ACSM in coastal locations. We have also added to this section that exploring the mechanism of sea salt interference within the instrument and how it differs from using a standard vaporizer would also be a valuable subject of further study.
Below we address the remaining comments individually.
Referee 1
Comments to the Author
The manuscript of “Interference of sea salt in capture vaporizer-ToF-ACSM measurements of biomass burning organic aerosols in coastal locations” by Sutresna et al. reports the interference of sea salt particles in ToF-ACSM equipped with the new capture vaporizer, and found that their fragmentation can affect the marker ions m/z 60 for biomass burning organic aerosols. The results are interesting and important to quantifying organic aerosols from different sources in coastal areas using CV-ToF-ACSM. However, the data quality control is not rigorous enough, and the present manuscript lacks substantial solutions or more in-depth analysis, for example, using the PMF source apportionment may distinguish between sea salt related OA and BBOA or not? Therefore, it is unpublishable at its current status before some questions have been well addressed.
Major comments:
1. The authors report the interference of sea salt on BBOA marker ions throughout the manuscript, but do not resolve BBOA from organic aerosols through any source apportionment method. According to the significant difference in the linear relationship between m/z 60 and m/z 73 affected by sea salt particles in Figure 2, I believe that sea salt related OA and BBOA can be distinguished through source apportionment methods such as positive matrix factorization (PMF). Have the authors attempted source apportionment of measured organic aerosols?
Response: In response to this comment, we have added Section 3.2 (“PMF”). Please refer to the response at the start of this document for further detail.
2. The authors believe that m/z 73 can fully indicate biomass burning due to its correlation with levoglucan and BB-related black carbon. I support this conclusion in strong biomass burning events. However, the Spearman correlation coefficients in Figure 3 represent a monotonic relationship but not linear relationship. Therefore, I do not think, this correlation can rigorously prove the indicative role of m/z 73.
Response: Thank you for raising this point, the following response has been added to the text in Section 3.1 (“m/z 60 vs. m/z 73”):
“While it might be reasonable to expect a linear relationship between a biomass burning marker ion and levoglucosan/BC_bb, the relationship between m/z 73 and levoglucosan/BC_bb does not have to be linear to be indicative of a positive correlation. In addition, when conducting a linear regression between m/z 73 and the BBOA marker species, there is nothing in the residuals that suggests that m/z 73 is not positively correlated with either species.”
3. Why is the f60/f73 in levoglucan spectrum higher than the f60/f73 in total OA measured during biomass burning events? Perhaps there are other sources for m/z 73 as well? Also, m/z 60 may also contain other ions besides biomass burning and sea salt.
Response: There is slight variation in the measurement of ions from instrument to instrument (even when different instruments both measure standards of the same species) that makes it possible for f60/f73 from the levoglucosan observed at both sites to differ somewhat from those measured in the standards.
While it is absolutely possible that there are other sources of m/z 73 and m/z 60, Figure 3 shows that m/z 73 is strongly associated with biomass burning aerosols, and by extension, m/z 60 is also strongly associated with biomass burning aerosols when it correlates well with m/z 73.
For reasons outlined in the response at the start of the document, this part of Section 3 is no longer in the paper.
4. The study of Hu et al. (2018) also reported some new biomass burning marker ions like C2H2+, C3H4O+, C5H4O+. Have the authors also discussed these?
Response: We agree that there is a need to investigate the alternative marker ions proposed by Hu et al. (2018), which will add valuable insight to our future work. We have added Section 6 (“Future work”) to address this.
5. There are many values less than 0 in m/z 60 and m/z 73 in Figure 2, please explain and handle these negative values properly. These seem to be related to the low OA concentration in Figure 3. Therefore, I doubt whether m/z 60 and m/z 73 can still be used at this time.
Response: While we appreciate the concern for the quality of the data, given that the magnitudes of the negative values are small and don’t have an impact on the implications of the paper, we think that they are indicative of periods of low total OA (including biomass burning OA) and do not need to be removed.
6. I’m curious, under what conditions will the interference of sea salt be significant? what conditions is biomass combustion dominant? Is it related to the direction of the airflow? If that's the case, backward trajectory analysis may be an effective support.
Response: From our investigations, we have found that interference from sea salt in CV-ACSM measurements are significant in locations close to the open ocean when biomass burning events occur. Airflow is related to whether biomass burning or sea salt is the dominant source and therefore back trajectory analysis would be a useful tool in explaining the contribution of both sources. In this paper, we are highlighting the occurrence of this interference, and more detailed source apportionment would need to be conducted in a further study involving back trajectory analysis.
Please also refer to the response at the start of this document.
Minor comments:
1. Methods section: What is the flow rate of CV-TOF-ACSM equipped with PM1 hole? To my knowledge, the TOF-ACSM flow rate for measuring PM2.5 is about 0.1L min-1.
Response: The flow rate for measuring PM1 is also similarly around 0.1 Lmin-1.
2. Please check the spaces between words in the full text.
Response: Thank you, this has been checked and corrected.
3. Methods section: Please explain the purpose of radon measurement.
Response: We agree with the need for this explanation. The following sentence has been added to the radon subsection of the Methods: “Radon is used as a marker for terrestrial air, and low radon concentrations are correlated with marine air and should be an indicator of elevated sea salt aerosol concentration.”
4. Results section: Table S1 lists many literatures about BBOA using CV-AMS or CV-ACSM, but there are too few reference values for f60/f73 in Table 1.
Response: Please refer to the response at the start of this document, which explains why references to f60/f73 ratio including Table 1 have been removed.
5. Results section: What is the detection limit of OA measured by CV-ToF-ACSM? Is the OA measurement of ~ng m-3 still accurate?
Response: The detection limit, which is calculated by 3 x standard deviation of measurements collected using a zero HEPA filter, calculated for total OA in this study was 186.7 ngm-3, but the detection limit can also be calculated for individual ions. The detection limit determined for m/z 73 was 4.2 ngm-3, and the majority of measurements involving biomass burning events saw m/z 73 concentrations above this level. These details have been added to the CV-ToF-ACSM segment of Section 2.2 (“Instrumental setup”) and the third paragraph of Section 3.1 (“m/z 60 vs. m/z 73”).
Referee 2
Comments on “Interference of sea salt in capture vaporizer-ToF-ACSM measurements of biomass burning organic aerosols in coastal locations” by Sutresna et al.
The organic ions of m/z 60 and m/z 73 are two makers for the biomass-burning derived OA(BBOA)in an aerosol mass spectrometer (AMS)/Aerosol chemical speciation monitor (ACSM), which was widely used in the world to measure the main chemical composition of fine particles. The authors show the interferences of sea-salt aerosols to these two makers during biomass burning plumes in the recently-developed time of flight ACSM coupled with a capture vaporizer. After reading through the manuscript, I believe the evidence for the interferences is solid, which shall be reported. However, several questions shall be clarified before the publication.
Major comments
1) The authors only focus on m/z 60 and 73. Multiple ions were enhanced in the spectrum of standard levoglucosan aerosols in CV-ToF-ACSM. Are there other ions that also show two distinguished regression slopes? If the answer is positive, then these ions might be also good biomass-burning makers in CV-ACSM. Especially the different correlations between other ions with m/z 73 and m/z 60, respectively can be good candidates.
Response: Other ions are well-correlated with m/z 73 as an established BBOA marker, e.g. m/z 55, which is a topic for further study as discussed in Section 6. Please also refer to the response at the start of this document.
2) I think the analysis of the manuscript can be stepped further. The authors shall also report the interferences of sea-salt on m/z 60 and 73 to PMF analysis of biomass burning OA, which is important for AMS users and is important to understand the influences of this interference.
Response: Please refer to the response at the start of this document which details the addition of Section 3.2 (“PMF”).
3) The authors reported this phenomenon of sea-salt interferences; however, the authors did not give a solution for these interferences. E.g., The quantification method to obtain mass concentration of biomass burning-derived m/z 60 and m/z 73 was not reported. As shown in Fig. 2a and d, in theory, the authors might be able to offset the interferences from sea-salt by using the correlation between m/z 60 and other sea-salt tracers (e.g., m/z 83, m/z 58, m/z 81).
Response: We agree that finding a solution to the interference observed in m/z 60 and quantifying the proportion of it from biomass burning is highly important, with the PMF solutions being a key step in achieving that. However, we believe that this paper should focus on identifying this interference along with some potential solutions, with the detailed characterisation of particle sources being its own study (as mentioned in the new Section 6 [“Future work”]).
With respect to m/z 73, that ion only comes from BBOA, so the threshold concentration for m/z 73 was identified as the point after which m/z 60 is strongly positively correlated with m/z 73 and is therefore likely to originate from BBOA.
Regarding alternative sea salt marker ions that could in theory be used to separate the contribution of m/z 60 from sea salt, ions such as m/z 58, m/z 81, and m/z 83 are also present in levoglucosan fragmentation (Figures S1 and S2) and therefore cannot be used to discriminate between sea salt and biomass burning.
Minor comments:
4) The radon did not show differences in mass concentration in the KCG site between the two slopes based on Fig.2f.
Response: While we acknowledge that the difference in colour representing the radon concentration between the points above and below the m/z 73 threshold is less visually distinct at KCG compared to COALA, we have conducted a pairwise t-test between the radon concentrations for points above and below the m/z 73 threshold and determined that there is a statistically significant difference between the two subsets. The p-value from the t-test of p < 0.001 has been quoted in the figure.
5) “This is because the capture vaporizer enables the detection of refractory particles 28 that include sea salt”; Not a capture vaporizer was used in the reference of 28
Response: Thank you, the reference has been amended to Mynard et al.
6) The first paragraph of Section 3 “results”. The figures were not referred to in the entire paragraph, which is confusing to read.
Response: This has been noted, references to all figures have been added to the first paragraph of Section 3 “Results”.
7) The second paragraph of Section 3 “results” Please specify what type of OA was reported here for the f60/f73 ratios. Standard levoglucosan or biomass-burning OA. The discussion here is unclear.
Response: While it appears that the second paragraph does mention that the f60/f73 ratio comes from levoglucosan standards, we have found that this clarification was not made in the caption for Table 1, which would cause similar confusion. However, for reasons explained in the response at the start of this document, we have removed Table 1 from the text.
Round 2
Revised manuscript submitted on 05 abr. 2024![](https://www.rsc-cdn.org/pubs-core/2022.0.148/content/NewImages/icon-letter.png)
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20-Apr-2024
Dear Mr Sutresna:
Manuscript ID: EA-ART-12-2023-000171.R1
TITLE: Interference of sea salt in capture vaporizer-ToF-ACSM measurements of biomass burning organic aerosols in coastal locations
Thank you for your submission to Environmental Science: Atmospheres, published by the Royal Society of Chemistry. I sent your manuscript to reviewers and I have now received their reports which are copied below.
I have carefully evaluated your manuscript and the reviewers’ reports, and the reports indicate that revisions are necessary.
Please submit a revised manuscript which addresses all of the reviewers’ comments. Further peer review of your revised manuscript may be needed. When you submit your revised manuscript please include a point by point response to the reviewers’ comments and highlight the changes you have made. Full details of the files you need to submit are listed at the end of this email.
Please submit your revised manuscript as soon as possible using this link:
*** PLEASE NOTE: This is a two-step process. After clicking on the link, you will be directed to a webpage to confirm. ***
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You should submit your revised manuscript as soon as possible; please note you will receive a series of automatic reminders. If your revisions will take a significant length of time, please contact me. If I do not hear from you, I may withdraw your manuscript from consideration and you will have to resubmit. Any resubmission will receive a new submission date.
The Royal Society of Chemistry requires all submitting authors to provide their ORCID iD when they submit a revised manuscript. This is quick and easy to do as part of the revised manuscript submission process. We will publish this information with the article, and you may choose to have your ORCID record updated automatically with details of the publication.
Please also encourage your co-authors to sign up for their own ORCID account and associate it with their account on our manuscript submission system. For further information see: https://www.rsc.org/journals-books-databases/journal-authors-reviewers/processes-policies/#attribution-id
Environmental Science: Atmospheres strongly encourages authors of research articles to include an ‘Author contributions’ section in their manuscript, for publication in the final article. This should appear immediately above the ‘Conflict of interest’ and ‘Acknowledgement’ sections. I strongly recommend you use CRediT (the Contributor Roles Taxonomy, https://credit.niso.org/) for standardised contribution descriptions. All authors should have agreed to their individual contributions ahead of submission and these should accurately reflect contributions to the work. Please refer to our general author guidelines https://www.rsc.org/journals-books-databases/author-and-reviewer-hub/authors-information/responsibilities/ for more information.
I look forward to receiving your revised manuscript.
Yours sincerely,
Dr Lin Wang
Associate Editor, Environmental Science: Atmospheres
Environmental Science: Atmospheres is accompanied by companion journals Environmental Science: Nano, Environmental Science: Processes and Impacts, and Environmental Science: Water Research; publishing high-impact work across all aspects of environmental science and engineering. Find out more at: http://rsc.li/envsci
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Reviewer 1
The authors have satisfactorily addressed the concerns I raised. The revised manuscript can now be accepted for publication.
Reviewer 2
Please see my comments in the attached document.
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Responses to reviewer comments:
We would like to again thank the referees for their further comments and suggestions. The suggestions have helped to clarify our findings in the PMF work, particularly in comments 1 and 2. While we have attempted to implement the suggestion in comment 3, we found that it would require further study to develop it into the optimal method of removing sea salt interference from the organics measurements. The details of this attempted implementation can be found in the response to comment 3.
1) For PMF factors, the names of “F1”, “F2” and “F3” are confusing. The PMF factors shall be named that can represent their sources. The source of a few factors is very clear. E.g., Sea Salt aerosols with pronounced m/z 58 and m/z 60, biomass-burning aerosols, oxygenated OA, etc.
Response:
Thank you for raising this issue, the names of the factors have been changed to reflect the particle sources in Section 3.2 (“PMF”), as well as in Figures S5, S6, 4, and 5.
2) the m/z 60 peaked with m/z 58(Na35Cl) is Na37Cl, which proved the ability of ToFACSM to measure sea salt aerosols. The question is how much of the m/z 60 comes from this factor?
The authors shall calculate the PMF factor contribution to m/z 60, m/z 58 and m/z 73. The results can clarify if the m/z 60/ enhancement is due to the sea salt aerosol. E.g., Figure 2 can also color code with the fraction of sea salt aerosol in total OA.
Response:
We agree that the text needs to include the proportions of m/z 58, 60, and 73 in each factor. This has been added to Section 3.2, as well as Figures S5 and S6. Figure 6 has been added to illustrate the distinct contribution of the sea salt factors in points below and above the m/z 73 threshold at both sites, as well as the following text:
“Lastly, shading the correlation plot between m/z 60 and m/z 73 with the percentage of Sea Salt factor concentration in total OA shows that the proportion of the Sea Salt factors are significantly higher in points below the m/z 73 threshold concentrations compared to above at both sites (Figure 6). At COALA, the mean percentage of Sea Salt was 8.90% below the threshold and 1.19% above (p < 0.001); while at KCG, the mean % of Sea Salt was 39.60% below the threshold and 0.64% above (p < 0.001).”
3) In the final results, if the m/z 58 was predominantly contributed by the Seasalt aerosol, then the ratio of m/z 60 and m/z 58 (0.31) can be used to correct the interferences of sea salt to ambient OA in the fragmentation table. The authors shall show the correlation between the corrected m/z 60 with m/z 73 to evaluate the correction.
Response:
We have attempted to separate the concentration of sea salt-60 using the fragmentation table as the referee suggested. The process was as follows:
• We created a new species called SS (sea salt) and assigned all m/z 58 concentration to that species
• frag_SS[60] = frag_SS[58] x 0.323 (the isotopic ratio between 35Cl and 37Cl used in the Tofware fragmentation table)
• frag_Org[60] = Total m/z 60 - frag_SS[60]
As seen in the updated Figures S5 and S6, the fraction of m/z 58 in each location’s sea salt factor are 63% in COALA and 93% at KCG.
At KCG, the resulting correlation between m/z 60 and m/z 73 weakens substantially from 0.77 in Figure 2 to 0.21. This is likely because there is a non-negligible amount of non-sea salt m/z 58 in the other factors, which leads to a large underestimation of non-sea salt m/z 60. The figure below [please refer to the figure in the comment response Word document]. compares the new correlation between m/z 60 and m/z 73 with the slope observed in the original m/z 60 vs m/z 73 correlation plot from points above the m/z 73 threshold (2.68), where the slope of the adjusted correlation is 0.28. It can also be observed by the points with the highest m/z 44 concentration falling to below 0 on the y-axis, as opposed to being around 0.025 in the original correlation plot.
This phenomenon is even more visible in COALA [shown in the comment responses Word document], where the proportion of non-sea salt m/z 58 is even higher and the reduction in apparent non-sea salt m/z 60 concentration is such that many of the points fall from 0.05 in the y-axis of the original correlation plot to well below 0. The original gradient of 1.97 also far exceeds the slope of the revised correlation plot of 0.36, while the correlation coefficient drops from 0.97 to 0.45.
While using the fragmentation table to correct for sea-salt m/z 60 using m/z 58 was a possible way to remove the influence of sea salt on organics concentrations, we found that the level of non-sea salt m/z 58 was too high and had too great an effect on the revised estimated non-sea salt m/z 60 to be an effective solution. Though we have decided not to include it in this paper, identifying corrections in the fragmentation table such as this is a valuable avenue for further study and has been added to Section 6 “Future Work”.
Round 3
Revised manuscript submitted on 03 may. 2024![](https://www.rsc-cdn.org/pubs-core/2022.0.148/content/NewImages/icon-letter.png)
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04-May-2024
Dear Mr Sutresna:
Manuscript ID: EA-ART-12-2023-000171.R2
TITLE: Interference of sea salt in capture vaporizer-ToF-ACSM measurements of biomass burning organic aerosols in coastal locations
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