the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Marine Carbohydrates and Other Sea Spray Aerosol Constituents Across Altitudes in the Lower Troposphere of Ny-Ålesund, Svalbard
Abstract. Marine combined carbohydrates in aerosol particles (CCHOaer) have the potential to influence cloud formation and properties, but it remains unclear to what extent they reach altitudes relevant for cloud processes. Balloon-borne measurements of major sea spray aerosol (SSA) constituents, including sodium (Na⁺aer) and CCHOaer, were conducted in autumn 2021 and spring 2022 in Ny-Ålesund (Svalbard). Total suspended particles were collected at 321–1112 m, covering both the marine boundary layer and the free troposphere, with Na⁺aer ranging 23–850 ng m-3 and CCHOaer 3.8–274 ng m-3. The chemical composition of balloon-borne aerosol samples was compared with synchronized ground level measurements at the balloon's winch (Na⁺aer: 35–3710 ng m-3; CCHOaer: 1.9–194 ng m-3), and at the Old Pier (Na⁺aer: 140–1470 ng m-3; CCHOaer: 1.6–10.0 ng m-3), where freshly emitted SSA particles were sampled. Surface seawater from the Kongsfjorden was analyzed to evaluate the sea-air transfer of marine CCHO. Air mass histories, atmospheric mixing, and cloud conditions were evaluated for three selected cases to explain vertical concentration patterns. A strong correlation (R=0.78, p<0.001) between combined xylose (<0.2–14.1 ng m-3) in CCHOaer and oxalateaer (<1–67 ng m-3) across all altitudes, suggests either coproduction or a connection through atmospheric processing. These results provide a first comprehensive picture of local primary sea-air transfer of marine combined carbohydrates and highlight the roles of long-range transport, in-situ formation, and chemical aging in shaping their atmospheric distribution.
Competing interests: At least one of the (co-)authors is a member of the editorial board of Atmospheric Chemistry and Physics.
Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims made in the text, published maps, institutional affiliations, or any other geographical representation in this paper. While Copernicus Publications makes every effort to include appropriate place names, the final responsibility lies with the authors. Views expressed in the text are those of the authors and do not necessarily reflect the views of the publisher.- Preprint
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Status: open (extended)
- RC1: 'Comment on egusphere-2025-4336', Anonymous Referee #1, 11 Nov 2025 reply
Data sets
Dissolved and particulate carbohydrates and inorganic ions in the sea surface microlayer and bulk water of Kongsfjorden (Autumn 2021/Spring 2022) S. Zeppenfeld and L. Schmidt https://doi.org/10.1594/PANGAEA.982606
Marine combined carbohydrates and inorganic ions in atmospheric total suspended particles across altitudes in the lower troposphere of Ny-Ålesund, Svalbard S. Zeppenfeld et al. https://doi.org/10.1594/PANGAEA.982703
HATPRO microwave radiometer measurements at AWIPEV, Ny-Ålesund (2019-2021) K. Ebell and C. Ritter https://doi.org/10.1594/PANGAEA.943004
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General comments:
The data set, focusing on carbohydrates in arctic aerosols at different altitudes in the atmosphere and samples of relevant depths from seawater, represents a valuable contribution, which is novel in its detail. Explicitly the high data coverage including autumn to spring months and the three showcases dissecting different meteorological and stratification scenarios are interesting. The manuscript makes a comprehensive contribution to disentangling the sources and role of carbohydrates present in primary marine aerosols, provided that the results and discussion are still appropriately revised. While the methods seem robust and are clearly outlined (however, I am not an expert in sampling aerosols nor in executing meteorological or trajectory calculations), I am not convinced by certain assumptions and interpretations, which are in particular drawn from case III. I would recommend to further include comparative figures and literature to evaluate concentration ranges and composition of CCHO. Overall, the manuscript is well structured and the language is appropriate.
With regards to the conclusions drawn from case III (high CCHO, calcium and magnesium concentrations versus lower sodium concentrations, samples influenced by cloud droplets) and the correlation between oxalate and xylose as discussed in chapter 3.3, I would suggest that the authors consider the following scenario. Elevated oxalate concentrations have been identified to correspond to the biological productive seasons above remote oceanic regions (Rinaldi et al., 2011), while xylose concentrations increase after certain phytoplankton blooms (Sperling et al., 2017). Marine aggregates, such as TEP composed of carbohydrates, also increase during blooms and are further relying on divalent cations such as Ca. Oxalate on the other hand, forms complexes with divalent cations including Ca (Furukawa and Takahashi, 2011), while oxalic acid increases hygroscopicity. In case III, aerosol particles were sampled within cloud water. Cloud water has been previously shown to exhibit a high number of TEP (van Pinxteren et al., 2022). As the authors stated, lower Na concentrations could be explained by previous wet precipitation (L528), while higher Ca and Mg concentration could result from the CCHO matrices excluding Na. I am thus not sure if the suggested secondary production pathway within the atmosphere is the most obvious/reasonable potential pathway explaining the data sets presented here.
Specific comments:
L68 The critical information here is that carbohydrates are a major product of photoautotrophic organisms, which represent the base of the food web. Carbohydrates can be rapidly consumed by heterotrophic organisms, however, in dependence of their structure and composition.
L362 I would recommend to group winch/pier and balloon samples into the corresponding categories: a) identical, b) lower at the ground, c) higher at the balloon and represent the categorized data in a corresponding plot (e.g. boxplots). It is complicated to track every single date and sodium concentration listed back to the timeseries (Figure 2) and then compare it to the corresponding CCHO concentration (and potentially composition) in aerosol particles (L485-498). Especially, because the authors later state that sodium and CCHO concentrations covaried (L495).
L443 As the results from the seawater analysis seem to be an integral part of your results and also the discussion would profit, I would include at least one comprehensive figure on seawater composition in the main manuscript and not only supplement.
In general, it would be very interesting to see a comparative figure of the (relative) carbohydrate composition from the seawater, over the pier and winch to higher altitudes (balloon). This would also enable the authors to better judge on the state of transformation (e.g. bacterial degradation) as comparative literature exists at least for oceanic profiles and mesocosm bloom studies (e.g. Goldberg et al., 2009; Engel, Harlay et al., 2012; Sperling et al., 2017; Hasenecz et al., 2020). Potentially further information could be revealed, which may assist with the interpretation of the three case studies.
L546 Again, the relative CCHO composition is not represented and would add a valuable contribution to the manuscript (see comment above).
L697 Sodium was markedly higher at the ground.
L711 This assumption sounds a little biased, see comments provided above and below with regards to the interpretation of results.
L721 I am not sure if atmospheric aging has been proven at this point. Potentially refer to 'atmospheric processing'. Differences in aging/ the residence time would also imply differences in source locations.
L771 As the model does not resolve the SML, which is frequently enriched as also stated by the authors, not crossing the marginal-ice zone does not necessarily imply no major oceanic contributions.
L788 'aerosolized taxa' refers to bacteria, which are commonly found in oceanic or terrestrial surfaces? Clarify.
L789 Many heterotrophic bacteria metabolize carbohydrates. Especially in the surface ocean, they rely heavily on primary products, including major fractions of carbohydrates, with phytoplankton production at the base of the food chain. I.e. if it is assumed that these bacteria were transferred from the ocean surface into aerosol particles, such metabolic characteristics are ordinary.
L864-865 This is only one side of the possible interpretation: Maybe xylose was only present in the CCHO of aerosol particles and not at all processed and/or released into the free fraction?
Technical corrections:
L72-73 Rephrase sentence as incomplete.
L721 If em-dashes are used instead of comma or brackets, please use a concise size etc. Their usage is rather unusual in a scientific context, and I would recommend to reduce them throughout the whole manuscript.
L402 Balloon (III) is two times mentioned in figure 2a and varies with altitude. Please clarify and include a statement in the figures caption.
L599 'both HALFBACs' As the sentence is very long, it is not clear until L604 if the comparisons are related to the balloon (III) and zeppelin (IV) observations in figure 3a or rather to ground and altitude samples, as specified only at the end. Clarify.