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Pre-deliquescent water uptake in deposited nanoparticles observed with in situ ambient pressure X-ray photoelectron spectroscopy

Lin, Jack J. and Raj R., Kamal and Wang, Stella and Kokkonen, Esko and Mikkelä, Mikko-Heikki and Urpelainen, Samuli and Prisle, Nønne L. (2021) Pre-deliquescent water uptake in deposited nanoparticles observed with in situ ambient pressure X-ray photoelectron spectroscopy. Atmospheric Chemistry and Physics, 21 (6). pp. 4709-4727. ISSN 1680-7324. doi:10.5194/acp-21-4709-2021.

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We study the adsorption of water onto deposited inorganic sodium chloride and organic malonic acid and sucrose nanoparticles at ambient water pressures corresponding to relative humidities (RH) from 0 % to 16 %. To obtain information about water adsorption at conditions which are not accessible with typical aerosol instrumentation, we use surface-sensitive ambient pressure X-ray photoelectron spectroscopy (APXPS), which has a detection sensitivity starting at parts per thousand. Our results show that water is already adsorbed on sodium chloride particles at RH well below deliquescence and that the chemical environment on the particle surface is changing with increasing humidity. While the sucrose particles exhibit only very modest changes on the surface at these relative humidities, the chemical composition and environment of malonic acid particle surfaces is clearly affected. Our observations indicate that water uptake by inorganic and organic aerosol particles could already have an impact on atmospheric chemistry at low relative humidities. We also establish the APXPS technique as a viable tool for studying chemical changes on the surfaces of atmospherically relevant aerosol particles which are not detected with typical online mass- and volume-based methods.

Item Type:Article
Related URLs:
URLURL TypeDescription
Lin, Jack J.0000-0002-4453-1263
Raj R., Kamal0000-0002-6437-316X
Wang, Stella0000-0003-4626-5875
Kokkonen, Esko0000-0002-3674-7486
Urpelainen, Samuli0000-0002-3734-0450
Prisle, Nønne L.0000-0002-2041-6105
Additional Information:© Author(s) 2021. This work is distributed under the Creative Commons Attribution 4.0 License. Published by Copernicus Publications on behalf of the European Geosciences Union. Received: 6 April 2020 – Discussion started: 29 April 2020; Revised: 1 February 2021 – Accepted: 3 February 2021 – Published: 26 March 2021. Code availability: The SPANCF fitting package is available from Edwin Kukk, Data availability: Data for the XPS spectra are available at (Prisle, 2021). Supplement: The supplement related to this article is available online at: Author contributions: Conceptualization, funding acquisition, supervision and project administration were performed by NLP. The experiments were carried out by JJL, KRR, SW, EK, MHM and SU. Data analysis was done by SU, JJL, SW and NLP. The first draft of the paper was written by JJL, SU and NLP with input from all co-authors. The authors' response was written by JJL, NLP and SU with input from all co-authors. The revised draft was written by JJL and NLP with input from all co-authors. The authors declare that they have no conflict of interest. We acknowledge MAX IV Laboratory for time on beamline SPECIES. Research conducted at MAX IV, a Swedish national user facility, is supported by the Swedish Research Council under contract 2018-07152, the Swedish Governmental Agency for Innovation Systems under contract 2018-04969 and Formas under contract 2019-02496. We warmly thank Jenny Rissler and Birgitta Svenningsson for assistance with preparation of samples and estimation of surface coverage. This project has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program, project SURFACE (grant agreement no. 717022). The authors also gratefully acknowledge the financial contribution from the Academy of Finland, including grant nos. 308238, 314175, 335649, 290145, 326291 and 331532. Review statement: This paper was edited by Thorsten Bartels-Rausch and reviewed by two anonymous referees.
Funding AgencyGrant Number
European Research Council (ERC)717022
Academy of Finland308238
Academy of Finland314175
Academy of Finland335649
Academy of Finland290145
Academy of Finland326291
Academy of Finland331532
Issue or Number:6
Record Number:CaltechAUTHORS:20210415-130954184
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Official Citation:Lin, J. J., Raj R, K., Wang, S., Kokkonen, E., Mikkelä, M.-H., Urpelainen, S., and Prisle, N. L.: Pre-deliquescent water uptake in deposited nanoparticles observed with in situ ambient pressure X-ray photoelectron spectroscopy, Atmos. Chem. Phys., 21, 4709–4727,, 2021
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:108746
Deposited By: Tony Diaz
Deposited On:16 Apr 2021 20:03
Last Modified:19 Apr 2021 16:13

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