From the journal Environmental Science: Atmospheres Peer review history

13-Jan-2023

Dear Dr Hill:

Manuscript ID: EA-ART-11-2022-000154
TITLE: Resolving the controls over the production and emission of ice-nucleating particles in sea spray

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.

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. ***

https://mc.manuscriptcentral.com/esatmos?link_removed

(This link goes straight to your account, without the need to log on to the system. For your account security you should not share this link with others.)

Alternatively, you can login to your account (https://mc.manuscriptcentral.com/esatmos) where you will need your case-sensitive USER ID and password.

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 Tzung-May Fu
Associate Editor
Environmental Science: Atmospheres
Royal Society of Chemistry

************

Reviewer 1

The authors design a series of experiments to explore the sources, conditions, and controls of marine ice-nucleating particles. By adding dead biomass of three diverse phytoplankton species to a marine aerosol generating tank, they showed INP production was stimulated by all species, and coincided with increases in nano flagellates and viruses. The study provides a new and valuable insight into INPs. I have outlined a few issues below that should be addressed prior to publication.

1. The authors pointed out that phytoplankton blooms appear to be large producers of INEs. The authors may quantify the contribution of Phytoplankton blooms to INEs in the remote ocean regions to strengthen the significance of this study.
2. The authors conducted the experiments based on a miniature Marine Aerosol Reference Tank filled with seawater. What extent is this representative of the real marine environment. Also, does the author consider the influence of meteorological factors?
3. Are there other factors besides phytoplankton types that might affect the production of INEs? The authors can add more relevant previous research results to the introduction.
4. Sea spray is one of the major global sources of atmospheric particles, what extent of these particles are capable of nucleating ice? It is clear that the contribution of real world sea spray to atmospheric aerosol and particularly to the INP fraction is a complex topic. The authors should elaborate the applicability of results from this study for atmospheric implications.
5. It is suggested to adjust the unified size of the picture in Fig 3 and expand the vertical range so that the error bar does not exceed the border of the graph.
6. Introduction: “there is a significant diversity in the representation of cloud phase and freezing processes, and their impact on climate”, add some references here.
7. Section 2.6: Did the authors correct the particle size spectra, including multiple charge correction and diffusion loss correction?

Reviewer 2

This paper investigates the ice nucleating particles in sea spray and how phytoplankton blooms collapse affects the ice nucleating entities and ice nucleating particles. To simulate the phytoplankton blooms collapse, authors added dead particulate biomass, diatom, and cyanobacterium to sea water to investigate the INP production as decomposition progresses. They tracked the bacterial and viral abundances during that time. The found interesting trend of INE during the duration of seven days of experiments. INE increased after few days and these INEs are mostly not heat labile. The authors provided suggestion about the origin of these entities. Another interesting experiment was addition of nutrient, the authors found INPs emission reduce significantly after the nutrient addition. The authors suggested the reason for decrease in INP is a monolayer is formed and displaced the sea surface microlayer. This is an interesting work and important contribution to the INP community. Overall, the manuscript is quite comprehensive and detailed. However, I feel some cases the text can be shorten and it would be easier for readers to follow the main message. Several details can be moved to supplementary information.
Minor comments:
I’m not sure if same sea water was used for all different experiments? If not how the composition, microbial activities and abundance change for different sea water?
Figure 2b is bit confusing as the authors use days as color gradient scale. I was wondering other plotting options would be easier to visualize, also is it possible to do same for INPs as well?
The observed INPs tends to peak earlier, and authors suggested that initially formed INEs had different characteristics and that may be responsible for the enrichment. Does author can hint what are those characteristics that may cause this?
The monolayer formation during the nutrient addition is interesting. The authors discussed about the altering the bubble bursting and reducing jet emission. What about any chemical mechanism? And if this is true for the DOC cocktail used in this study and if it would change for other nutrients?
The authors conducted the experiments for 7 days, what would the authors expect to happen to INE and INPs after that?

[This text has been copied from the PDF response to reviewers and does not include any figures, images or special characters.]

REVIEWER REPORT(S):

Reviewer 1
Comments to the Author
The authors design a series of experiments to explore the sources, conditions, and controls of marine ice-nucleating particles. By adding dead biomass of three diverse phytoplankton species to a marine aerosol generating tank, they showed INP production was stimulated by all species, and coincided with increases in nanoflagellates and viruses. The study provides a new and valuable insight into INPs. I have outlined a few issues below that should be addressed prior to publication.

Our thanks to Reviewer 1 for this generous overall summary.

1. The authors pointed out that phytoplankton blooms appear to be large producers of INEs. The authors may quantify the contribution of Phytoplankton blooms to INEs in the remote ocean regions to strengthen the significance of this study.

This is indeed the essential next step: to advance from mesocosm-based experiments to field studies of seawater in situ. At the moment, however, as we state in the Conclusions, “in the ocean, algae are often nutrient depleted and the bacterial degradation of algal detritus may create a different molecular fingerprint, affecting INE emissions differently than observed here”, which we have extended:

We should note that in the ocean algae are often nutrient depleted and the bacterial degradation of algal detritus may create a different molecular fingerprint, affecting INE emissions differently than observed here. Hence, it would be premature to extrapolate from this and similar studies to estimate INE production in situ.

INE concentrations in remote ocean regions do exhibit a wide range of values (Fig. 1), indicative of dynamic production and degradation/removal processes and, hence, the likelihood of correlations with biological markers such as protists.


Fig. 1. INEs in seawater from remote sites. All values have been corrected (+2 °C) to account for freezing point depression.

However, while many studies have shown that INE production is associated with blooms, since INPs peak in the decline phase, a simple correlation between Chl a and INEs will be offset/displaced in both time and space (moved downstream by currents). Hence, no clear link between the two has been found (Irish et al., 2017; McCluskey et al., 2018; Creamean et al., 2019; Irish et al., 2019; Hartmann et al., 2021). In the Southern Ocean (SO), the only measures of INEs are by McCluskey et al. (2018), south of Tasmania, which found consistently very low INE concentrations (Fig. 1), perhaps because Chl a levels indicated the region was experiencing a sustained bloom.

Any study aiming to quantify the contribution of phytoplankton blooms to INEs in situ needs to sample within a bloom repeatedly within the water mass as the bloom peaks and then declines. For example, there are several regions in the SO where very large blooms occur predictably every spring and summer, fertilized by upwellings or upward mixing of nutrients, especially iron and silicate, where currents interact with continental shelves, islands and even hydrothermal vents (Robinson et al., 2016; Schine et al., 2021). If caused by an island, peak Chl a occurs in a relatively stationary location downstream of it, decaying away as the progressively nutrient-depleted water advects away or is diluted by deepening of the surface mixed layer (Robinson et al., 2016). Alternatively, because the peak Chl a zone is relatively stationary, water within and downstream of the average bloom track could be sampled repeatedly to obtain longer-term averages.

A discussion of the possible role of blooms has been added to a paragraph of atmospheric implications, as the Reviewer has requested below.


2. The authors conducted the experiments based on a miniature Marine Aerosol Reference Tank filled with seawater. What extent is this representative of the real marine environment. Also, does the author consider the influence of meteorological factors?

The referee makes a good point. Any micro/mesocosm or wave channel experiment can never truly replicate the water body from which it was withdrawn, and since we cannot assess how much the artifacts that are introduced will modify the responses, until field studies are carried out the results must be considered indicative.

Having said that, we strived to preserve the seawater in its original state as much as allowed by the experimental design. For example, seawater samples were:
• flown to us overnight in sterile containers.
• the miniMART was pre-cleaned and rinsed with methanol before being dried and rinsed with 0.2 µm-filtered DI water. And once sealed the headspace was flushed with Hepa-filtered air. Effectiveness of these precautions to prevent colonization by terrestrial bacteria was supported by sequencing, which confirmed that all bacteria present at >0.1% relative abundance were of marine origin.
• The miniMART design generates SSA with a realistic aerosol distribution in a natural (i.e., gentle) manner that facilitates growth of microbial communities irrespective of their delicacy.

Necessarily, other aspects of the incubations required modifying the samples:
• Samples were filtered to remove phytoplankton (to prevent them producing fresh organic matter via photosynthesis) and larger protists (to prevent them consuming and altering the standing population of bacteria).
• The water was incubated somewhat warmer than ocean temperatures.

The INE response was consistent with other mesocosm/waveflume incubations (Wang et al., 2015; DeMott et al., 2016; McCluskey et al., 2017, 2018), as well as with observations in natural settings (Schnell and Vali, 1975; Trueblood et al., 2021).

We could not consider meteorological factors due to the nature of the enclosed mesocosm, but the device does automatically reproduce the aerosol produced by small whitecaps. We have added the following sentence to the Methods section.

The miniMART uses a plunging water jet, which replicates the bubble plumes generated by small waves, and so simulates the meteorological conditions consistent with the occurrence of small whitecaps generated by wind speeds >~3 m s−1.


3. Are there other factors besides phytoplankton types that might affect the production of INEs? The authors can add more relevant previous research results to the introduction.

Yes, the referee is correct, there are more variables that may directly or indirectly affect INE production. Additional factors shown to influence the INE loading in surface waters have been added to the Introduction, as indicated below.

Accordingly, INP concentrations over oceans are typically two or more orders of magnitude lower than over land.3,15,31,32 However, significant and sometimes “phenomenally active”27 excursions from typical background values in seawater and/or boundary layer air have been recorded, associated with a range of factors, such as higher concentrations of biological material, both dissolved22,23,29,32,33 and particulate (e.g., gel-like particles),27,32,33 enhanced productivity in upwelling regions,33−35 and a reduction in salinity caused by melting sea ice.22,23 Phytoplankton blooms appear to be large producers of INEs, especially during the microbial succession of bacteria, viruses and protists that ensues when they collapse and their organic matter is re-worked and decomposed.3,24,28,36−38,35 Emissions of INPs in sea spray aerosol (SSA) are also modulated by their enrichment in the sea surface microlayer (SML)21,23,24,29,39,37 and by the ratio of jet to film drop production, with the former being a more effective INE ejector.40,cf.,37 Other factors that may enhance INEs in surface waters include deposited dust35,44 and its stimulation of biological activity via iron fertilization.35

4. Sea spray is one of the major global sources of atmospheric particles, what extent of these particles are capable of nucleating ice? It is clear that the contribution of real world sea spray to atmospheric aerosol and particularly to the INP fraction is a complex topic. The authors should elaborate the applicability of results from this study for atmospheric implications.

We assume the referee is inquiring about the ice nucleating activity of pure sea spray (i.e., the salts) in the absence of organic ice nucleators. While sea salt is not known to be ice nucleation active in the temperature regime studied here (Wagner et al., 2018; Patnaude et al., 2021), at temperatures relevant to cirrus clouds laboratory significant fractions of SSA initiate heterogeneous freezing below ~-50°C, attributable to the crystalline NaCl and NaCl∙2H2O core (Schill and Tolbert, 2014; Wagner et al., 2018; Patnaude et al., 2021).

Nascent sea spray is also a low-efficiency INP, so accordingly we have added the following sentence to the Introduction:

Sea spray aerosol (SSA) is also a low efficiency ice nucleator compared with mineral dust.15,32


With regard to atmospheric implications, we want to avoid speculative over-reach, and so we have added a succinct paragraph to the Conclusions.

If phytoplankton blooms consistently generate and emit INPs, their atmospheric contribution would be most pronounced in remote regions of the SO.2 Chl a concentrations range widely (annual mean >0.1 to >2 mg m-3) across the SO,119 with a timing, scale, and biomass varying latitudinally and regionally. Latitudinally, blooms are driven by sunlight: in temperate “bioregions”, phytoplankton blooms occur in October, whereas near Antarctica they peak in January/February.119 In regions where currents interact with continental shelves, islands and hydrothermal vents, large blooms develop every spring and summer, fertilized by upwelling of nutrients, especially iron and silicate.120,121 Some marine and phytoplankton bloom-induced INEs/INPs can possess activity at the exceptionally warm temperatures required for secondary ice multiplication,21,33,36,108 a process that can generate ice particle concentrations orders of magnitude higher than the numbers of INPs present.


5. It is suggested to adjust the unified size of the picture in Fig 3 and expand the vertical range so that the error bar does not exceed the border of the graph.

The widths of the graphs in Fig. 3 vary intentionally in order to keep the spacing of each day length equal, as a guide to aid comparisons of changes with time. However, the Native DOC Control graphs were not sized correctly and have been fixed.

Error bars that exceed the borders of the graphs extend to zero, which cannot be shown on the log scale. We have added the following note in the figure legend.

Error bars that exceed the borders of the graphs extend to zero.


6. Introduction: “there is a significant diversity in the representation of cloud phase and freezing processes, and their impact on climate”, add some references here.

References have been added, including an extra one:

Gettelman, A., Bardeen, C. G., McCluskey, C. S., Järvinen, E., Stith, J., Bretherton, C., McFarquhar, G., Twohy, C., D'Alessandro, J., and Wu, W. 2020. Simulating observations of Southern Ocean clouds and implications for climate. Journal of Geographical Research: Atmospheres, 125, e2020JD032619. https://doi.org/10.1029/2020JD032619


7. Section 2.6: Did the authors correct the particle size spectra, including multiple charge correction and diffusion loss correction?

Yes, both multiple charge and diffusion loss corrections were applied to the SMPS particle size distributions generated in TSI’s Aerosol Instrument Manager (AIM) software.

 

Reviewer 2
Comments to the Author
This paper investigates the ice nucleating particles in sea spray and how phytoplankton blooms collapse affects the ice nucleating entities and ice nucleating particles. To simulate the phytoplankton blooms collapse, authors added dead particulate biomass, diatom, and cyanobacterium to sea water to investigate the INP production as decomposition progresses. They tracked the bacterial and viral abundances during that time. The found interesting trend of INE during the duration of seven days of experiments. INE increased after few days and these INEs are mostly not heat labile. The authors provided suggestion about the origin of these entities. Another interesting experiment was addition of nutrient, the authors found INPs emission reduce significantly after the nutrient addition. The authors suggested the reason for decrease in INP is a monolayer is formed and displaced the sea surface microlayer. This is an interesting work and important contribution to the INP community. Overall, the manuscript is quite comprehensive and detailed. However, I feel some cases the text can be shorten and it would be easier for readers to follow the main message. Several details can be moved to supplementary information.

We thank Reviewer 2 for their positive judgement, especially in appreciating the implications of the finding of BSA’s suppression of emissions via its displacement of the natural SML. As the Reviewer notes, we did aim to make the manuscript comprehensive and detailed, but we agree that it could be compacted to make it easier to follow the main message.

One section that we have reduced is 3.2.2 Heterotrophic bacterial composition and emissions during the N. atomus addition experiment. As can be seen, explanations for the dominance of the three most abundant OTUs have been moved to Table S2 in the ESI. If desired, Fig. 4, which shows the changes in relative abundances in water and SSA, can also be placed in the ESI.

Secondly, excessive detail in section 3.3 Pure nutrient addition experiment has been cut.

Thirdly, we have compacted the discussion of enrichment factors in section 3.4 Controls over INP emissions.


Minor comments:
1. I’m not sure if same sea water was used for all different experiments? If not how the composition, microbial activities and abundance change for different sea water?

Each incubation, by necessity, had to use a different starting batch of natural seawater (but sampled at the same location), which will have introduced some variation. The initial bacterial diversity/evenness in each sample will have been strongly modified as a result of rapid growth of bacteria possessing the heterotrophic niche space/ability to exploit the substrate added. For example, in the N. atomus detritus addition experiment, the community became dominated by around a dozen OTUs from three (expected) phylogenetic groups. Particular strains and species of viruses and nanoflagellates will, in turn, have been advantaged by the species of bacteria that proliferated.

Therefore, as a result of this strong selection for rapidly growing heterotophic (r selected) bacteria, it’s reasonable to expect that the outcome of each incubation would be broadly repeatable if replicated. The following elucidation has been placed in the ESI, in the header to Table S2, but can be moved to the main paper if desired.

Each incubation used a different starting batch of seawater (sampled at the same location). The initial bacterial diversity/evenness in each sample will have been strongly modified as a result of rapid growth of bacteria possessing the heterotrophic niche space/ability to exploit the substrate added. Viruses and nanoflagellates will, in turn, have been selected by the species of bacteria that proliferated. Due to this strong selection for rapidly growing heterotrophic bacteria, it’s reasonable to expect that the outcome of each incubation would be similar if replicated.


2. Figure 2b is bit confusing as the authors use days as color gradient scale. I was wondering other plotting options would be easier to visualize, also is it possible to do same for INPs as well?

We agree. We’ve made it clearer by simply using day number. Unfortunately, the lack of measures of HNF in the SSA for two of the experiments prevents us from making a similar summary for INPs.


3. The observed INPs tends to peak earlier, and authors suggested that initially formed INEs had different characteristics and that may be responsible for the enrichment. Does author can hint what are those characteristics that may cause this?

We have suggested that INE hydrophobicity may have played a role, but in fact we suspect that SML development, as the detritus was fragmented and decomposed, may have been the driving factor behind enhanced INP emissions. However, we have no evidence for either mechanism.


4. The monolayer formation during the nutrient addition is interesting. The authors discussed about that altering the bubble bursting and reducing jet emission. What about any chemical mechanism?

The reviewer raises a good point. It is also possible INEs adsorbed onto or formed aggregates/flocs with the BSA proteins. The following sentence has been added to that section.

Finally, it is possible that the BSA bound directly to the INEs, forming flocs too large to be ejected.

And if this is true for the DOC cocktail used in this study and if it would change for other nutrients?

Yes, while the potential was there when the natural detritus was added this was minimized by washing of the detritus before addition to remove the dissolved cellular fraction.


5. The authors conducted the experiments for 7 days, what would the authors expect to happen to INE and INPs after that?

In the control experiment, we did set up a separate test of INE persistence (Fig. 2). The first measure was made at the end of the miniMART incubation but had levels 3-5 times lower than in the miniMART (for unknown reasons). INE concentrations remained steady over the next 3 days, and then declined modestly over 3.5 months indicating either that the INEs were resistant to decomposition or that there was a dynamic equilibrium of production and decomposition. Because this was an informal test, we didn’t refer to it in the paper.


Fig. 2. INE persistence in a batch of the same seawater used in the control experiment. 500 mL was placed in a sterile container and constantly aerated (topped up with filter-sterilized DI water when needed). The INE concentrations measured in this container were on 30th Aug, 3rd Sept and 16th Dec.


New references
18. Gettelman, A., Bardeen, C. G., McCluskey, C. S., Järvinen, E., Stith, J., Bretherton, C., McFarquhar, G., Twohy, C., D'Alessandro, J., and Wu, W. 2020. Simulating observations of Southern Ocean clouds and implications for climate. J. Geophys. Res.: Atmos., 125, e2020JD032619. https://doi.org/10.1029/2020JD032619

32. Kanji, Z. A., Ladino, L. A., Wex, H., Boose, Y., Burkert-Kohn, M., Cziczo, D. J. and Krämer, M.: Overview of ice nucleating particles, Meteorological Monographs, 58, pp.1.1-1.33, https://doi.org/10.1175/AMSMONOGRAPHS-D-16-0006.1, 2017.

35. Trueblood, J. V., Nicosia, A., Engel, A., Zäncker, B., Rinaldi, M., Freney, E., Thyssen, M., Obernosterer, I., Dinasquet, J., Belosi, F. and Tovar-Sánchez, A.: A two-component parameterization of marine ice-nucleating particles based on seawater biology and sea spray aerosol measurements in the Mediterranean Sea, Atmos. Chem. Phys., 21, 4659-4676, https://doi.org/10.5194/acp-21-4659-2021, 2021.

44. Cornwell, G. C., Sultana, C. M., Prank, M., Cochran, R. E., Hill, T. C., Schill, G. P., DeMott, P. J., Mahowald, N. and Prather, K. A.: Ejection of dust from the ocean as a potential source of marine ice nucleating particles, J. Geophys. Res.: Atmos., e2020JD033073, https://doi.org/10.1029/2020JD033073, 2020.

119. Ardyna, M., Claustre, H., Sallée, J.-B., D’Ovidio, F., Gentili, B., van Dijken, G. , D’Ortenzio, F., and Arrigo, K. R.: 2017. Delineating environmental control of phytoplankton biomass and phenology in the Southern Ocean, Geophys. Res. Lett., 44, 5016–5024, https://doi.org/10.1002/2016GL072428, 2017.

120. Robinson, J., Popova, E. E., Srokosz, M. A., and Yool, A.: A tale of three islands: Downstream natural iron fertilization in the Southern Ocean, J. Geophys. Res.: Oceans, 121, 3350–3371, https://doi.org/10.1002/2015JC011319, 2016.

121. Schine, C. M. S., Alderkamp, A.-C., van Dijken, G., Gerringa, L. J. A., Sergi, S., Laan, P., van Haren, H., van de Poll, W. H. and Arrigo, K. R.: Massive Southern Ocean phytoplankton bloom fed by iron of possible hydrothermal origin. Nat. Comm., 12, 1211, https://doi.org/10.1038/s41467-021-21339-5, 2021.


Other references

Beall, C. M., T. C. J Hill, P. J. DeMott, T. Köneman, M. Pikridas, F. Drewnick, H. Harder, C. Pöhlker, J. Lelieveld, B. Weber, M. and Iakovides, M. 2022. Ice-nucleating particles near two major dust source regions. Atmospheric Chemistry and Physics, 22, 12607-12627.

Creamean, J. M., Cross, J. N., Pickart, R., McRaven, L., Lin, P., Pacini, A., Hanlon, R., Schmale, D. G., Ceniceros, J., Aydell, T., Colombi, N., Bolger, E., and DeMott, P. J.: Ice nucleating particles carried from below a phytoplankton bloom to the Arctic atmosphere, Geophys. Res. Lett., 46, 8572–8581, https://doi.org/10.1029/2019GL083039, 2019.

DeMott, P. J., Hill, T. C. J., McCluskey, C. S., Prather, K. A., Collins, D. B., Sullivan, R. C., Ruppel, M. J., Mason, R. H., Irish, V. E., Lee, T., Hwang, C. Y., Rhee, T. S., Snider, J. R., McMeeking, G. R., Dhaniyala, S., Lewis, E. R., Wentzell, J. J. B., Abbatt, J., Lee, C., Sultana, C. M., Ault, A. P., Axson, J. L., Diaz Martinez, M., Venero, I., Santos-Figueroa, G., Stokes, M. D., Deane, G. B., Mayol-Bracero, O. L., Grassian, V. H., Bertram, T. H., Bertram, A. K., Moffett, B. F., and Franc, G. D.: Sea spray aerosol as a unique source of ice nucleating particles, Proc. Natnl. Acad. Sci., 113, 5797–5803, http://dx.doi.org/10.1073/pnas.1514034112, 2016.

Gong, X., Wex, H., Pinxteren, M. V., Triesch, N., Fomba, K. W., Lubitz, J., Stolle, C., Robinson, T. B., Müller, T., Herrmann, H. and Stratmann, F. 2020. Characterization of aerosol particles at Cabo Verde close to sea level and at the cloud level–Part 2: Ice-nucleating particles in air, cloud and seawater. Atmospheric Chemistry and Physics, 20, 1451-1468.

Hartmann, M., Gong, X., Kecorius, S., van Pinxteren, M., Vogl, T., Welti, A., Wex, H., Zeppenfeld, S., Herrmann, H., Wiedensohler, A., and Stratmann, F.: Terrestrial or marine–indications towards the origin of ice-nucleating particles during melt season in the European Arctic up to 83.7° N, Atmos. Chem. Phys., 21, 1613–11636, http://dx.doi.org/10.5194/acp-21-11613-2021, 2021.

Irish, V. E., Elizondo, P., Chen, J., Chou, C., Charette, J., Lizotte, M., Ladino, L. A., Wilson, T. W., Gosselin, M., Murray, B. J., and Polishchuk, E.: Ice-nucleating particles in Canadian Arctic sea-surface microlayer and bulk seawater, Atmos. Chem. Phys., 17, 10583–10595, http://dx.doi.org/10.5194/acp-17-10583-2017, 2017.

Irish, V. E., Hanna, S. J., Yu, X., Boyer, M., Polishchuk, E., Ahmed, M., Chen, J., Abbatt, J. P., Gosselin, M., Chang, R., Miller, L. A., and Bertram, A. K.: Revisiting properties and concentrations of ice-nucleating particles in the sea surface microlayer and bulk seawater in the Canadian Arctic during summer, Atmos. Chem. Phys., 19, 7775–7787, http://dx.doi.org/10.5194/acp-19-7775-2019, 2019.

McCluskey, C. S., Hill, T. C. J., Malfatti, F., Sultana, C. M., Lee, C., Santander, M. V., Beall, C. M., Moore, K. A., Cornwell, G. C., Collins, D. B., Prather, K. A., Jayarathne, T., Stone, E. A., Azam, F., Kreidenweis, S. M., and DeMott, P. J.: A dynamic link between ice nucleating particles released in nascent sea spray aerosol and oceanic biological activity during two mesocosm experiments, J. Atmos. Sci., 74, 151–166, http://dx.doi.org/10.1175/JAS-D-16-0087.1, 2017.

McCluskey, C. S., Hill, T. C. J., Sultana, C. M., Laskina, O., Trueblood, J., Santander, M. V., Beall, C. M., Michaud, J. M., Kreidenweis, S. M., Prather, K. A., Grassian, V. H., and DeMott, P. J.: A mesocosm double feature: Insights into the chemical make-up of marine ice nucleating particles, J. Atmos. Sci., 75, 2405–2423, http://dx.doi.org/10.1175/JAS-D-17-0155.1, 2018.

Patnaude, R., R. J. Perkins, S. M. Kreidenweis and P. J. DeMott, Is ice formation by sea spray particles at cirrus temperatures controlled by crystalline salts? ACS Earth and Space Chemistry, 5, 2196–2211.

Schill, G. P. and Tolbert, M. A. 2014. Heterogeneous ice nucleation on simulated sea-spray aerosol using Raman Microscopy. J. Phys. Chem. C, 118, 29234–29241.

Schnell, R. C. and Vali, G. 1975. Freezing nuclei in marine waters. Tellus, 27, 321-323.

Wagner, R., J. Kaufmann, O. Möhler, H. Saathoff, M. Schnaiter, R. Ullrich, and T. Leisner. 2018. Heterogeneous Ice Nucleation Ability of NaCl and Sea Salt Aerosol Particles at Cirrus Temperatures. J. Geophys. Res.: Atmos., 123, 2841−2860.

Wang, X., Sultana, C. M., Trueblood, J., Hill, T. C. J., Malfatti, F., Lee, C., Laskina, O., Moore, K. A., Beall, C. M., McCluskey, C. S., Cornwell, G. C., Zhou, Y., Cox, J. L., Pendergraft, M. A., Santander, M. V., Bertram, T. H., Cappa, C. D., Azam, F., DeMott, P. J., Grassian, V. H., and Prather, K. A.: Microbial control of sea spray aerosol composition: A tale of two blooms, ACS Cent. Sci., 1, 124–131, https://doi.org/10.1021/acscentsci.5b00148, 2015.

20-Apr-2023

Dear Dr Hill:

Manuscript ID: EA-ART-11-2022-000154.R1
TITLE: Resolving the controls over the production and emission of ice-nucleating particles in sea spray

Thank you for submitting your revised manuscript to Environmental Science: Atmospheres. I am pleased to accept your manuscript for publication in its current form. I have copied any final comments from the reviewer(s) below.

You will shortly receive a separate email from us requesting you to submit a licence to publish for your article, so that we can proceed with the preparation and publication of your manuscript.

You can highlight your article and the work of your group on the back cover of Environmental Science: Atmospheres. If you are interested in this opportunity please contact the editorial office for more information.

Promote your research, accelerate its impact – find out more about our article promotion services here: https://rsc.li/promoteyourresearch.

We will publicise your paper on our Twitter account @EnvSciRSC – to aid our publicity of your work please fill out this form: https://form.jotform.com/211263048265047

How was your experience with us? Let us know your feedback by completing our short 5 minute survey: https://www.smartsurvey.co.uk/s/RSC-author-satisfaction-energyenvironment/

By publishing your article in Environmental Science: Atmospheres, you are supporting the Royal Society of Chemistry to help the chemical science community make the world a better place.

With best wishes,

Dr Tzung-May Fu
Associate Editor
Environmental Science: Atmospheres
Royal Society of Chemistry

Reviewer 1

The authors have addressed most of the concerns from the reviewer.