the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Molecular composition and processing of aqueous secondary organic aerosol in cloud at a mountain site in southeastern China
Abstract. Aqueous secondary organic aerosol (aqSOA) contributes substantially to organic aerosol (OA), affecting air quality, human health, and climate. However, the molecular composition and processing of aqSOA in cloud remain unclear due to limited online field measurements. We measured molecular composition of OA online (time resolution 20 s) and tracked its processing at a mountain site in southeastern China, using an Extractive ElectroSpray Ionization inlet coupled with a Time-of-Flight Mass Spectrometer (EESI-ToF-MS). We identified 2084 molecular formulas and compared OA composition from three sample types with adjacent time (<2 h): cloud droplets (CD), interstitial aerosol (INT), and cloud-free aerosol (CF) in representative cloud episodes. CHO class was the dominant constituent, followed by CHON class. The fraction of CHO was lower in CD than that in INT and CF, while the fraction of CHON was higher, which may result from the uptake of organonitrates or nitration in cloud water. Compounds in CD had more carbon, oxygen, and nitrogen number but lower O/C than INT and CF, which is attributed to accretion reactions in cloud water. We identified aqSOA tracers, including 39 new compounds, which were significantly enriched in CD compared with CF. This study also reveals rapid changes of aqSOA composition, which highlight the necessity for high time resolution measurement to capture the processing of aqSOA in cloud. Overall, this study provides clear information of processing of aqSOA in cloud and highlights the importance of accretion reactions, which has implications on the composition and physicochemical properties of SOA.
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 (until 29 Oct 2025)
- RC1: 'Comment on egusphere-2025-4322', Anonymous Referee #1, 02 Oct 2025 reply
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This manuscript reports high–time/mass resolution online molecular measurements of OA using EESI-TOF at a mountain site in SE China, comparing cloud droplets, interstitial, and cloud-free aerosol. It is clearly within ACP’s scope, addressing atmospheric composition and processes with implications for aerosol–cloud interactions and climate. However, the discussion of “tracers” requires more caution: the manuscript should clearly distinguish between true tracers and compounds showing enhanced signals, define the concept explicitly as illustrated below.
Major comments:
Minor comments:
Line 61: “Aerosol Mass Spectrometer (AMS) or Aerodyne Aerosol Chemical Speciation Monitor (ACSM)”.
Line 82: revise to “…at the summit of Damaojian Mountain, located in Jinhua City, Zhejiang Province, China.”
Line 105: delete “Here is a brief introduction.”, too informal.
Line 115: “signal-to-background ration (s/b)”.
Line 268: “To the best of our knowledge, this is the first observation of C16H48O8Si8 …”. As mentioned in major comments 2, the description needs to be considered.
Line 308: hours to a day.