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Molecular Composition and Volatility of Nucleated Particles from α-Pinene Oxidation between -50 °C and +25 °C

Ye, Qing and Kim, Changhyuk and Flagan, Richard (2019) Molecular Composition and Volatility of Nucleated Particles from α-Pinene Oxidation between -50 °C and +25 °C. Environmental Science and Technology, 53 (21). pp. 12357-12365. ISSN 0013-936X. doi:10.1021/acs.est.9b03265.

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We use a real-time temperature-programmed desorption chemical-ionization mass spectrometer (FIGAERO–CIMS) to measure particle-phase composition and volatility of nucleated particles, studying pure α-pinene oxidation over a wide temperature range (−50 °C to +25 °C) in the CLOUD chamber at CERN. Highly oxygenated organic molecules are much more abundant in particles formed at higher temperatures, shifting the compounds toward higher O/C and lower intrinsic (300 K) volatility. We find that pure biogenic nucleation and growth depends only weakly on temperature. This is because the positive temperature dependence of degree of oxidation (and polarity) and the negative temperature dependence of volatility counteract each other. Unlike prior work that relied on estimated volatility, we directly measure volatility via calibrated temperature-programmed desorption. Our particle-phase measurements are consistent with gas-phase results and indicate that during new-particle formation from α-pinene oxidation, gas-phase chemistry directly determines the properties of materials in the condensed phase. We now have consistency between measured gas-phase product concentrations, product volatility, measured and modeled growth rates, and the particle composition over most temperatures found in the troposphere.

Item Type:Article
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URLURL TypeDescription
Ye, Qing0000-0003-3797-8988
Kim, Changhyuk0000-0002-8744-4880
Flagan, Richard0000-0001-5690-770X
Additional Information:© 2019 American Chemical Society. Received: May 31, 2019; Revised: September 20, 2019; Accepted: September 25, 2019; Published: September 25, 2019. We thank the European Organization for Nuclear Research (CERN) for supporting CLOUD with important technical and financial resources. This research has received funding from the U.S. National Science Foundation under grants AGS-1801574, AGS-1801897, AGS-1649147, and AGS-1602086; the EC Horizon 2020 Programme (Marie-Sklodowska-Curie Innovative Training Network “CLOUD-MOTION” No. 764991); European Union Horizon 2020 programme MC–COFUND Grant 665779; German Federal Ministry of Education and Research (No. 01LK1601A); ERC-Consolidator Grant NANODYNAMITE 616075; Horizon 2020 Marie Sklodowska-Curie Grant 656994 (Nano-CAVa); ERC Advanced “ATM-GP” grant No. 227463; and the Swiss National Science Foundation Project 20FI20_159851, 200021_169090, 200020_172602 and 20FI20_172622. The FIGAERO–CIMS was supported by an MRI grant for the U.S. NSF AGS-1531284 as well as the Wallace Research Foundation. Q.Y. was supported by a Faculty for the Future Fellowship from the Schlumberger Foundation. The authors declare no competing financial interest.
Funding AgencyGrant Number
Marie Curie Fellowship764991
Marie Curie Fellowship665779
Bundesministerium für Bildung und Forschung (BMBF)01LK1601A
European Research Council (ERC)616075
Marie Curie Fellowship656994
European Research Council (ERC)227463
Swiss National Science Foundation (SNSF)20FI20 159851
Swiss National Science Foundation (SNSF)200021 169090
Swiss National Science Foundation (SNSF)200020 172602
Swiss National Science Foundation (SNSF)20FI20 172622
Wallace Research FoundationUNSPECIFIED
Schlumberger FoundationUNSPECIFIED
Issue or Number:21
Record Number:CaltechAUTHORS:20190925-160827651
Persistent URL:
Official Citation:Molecular Composition and Volatility of Nucleated Particles from α-Pinene Oxidation between −50 °C and +25 °C. Qing Ye, Mingyi Wang, Victoria Hofbauer, Dominik Stolzenburg, Dexian Chen, Meredith Schervish, Alexander Vogel, Roy L. Mauldin, Rima Baalbaki, Sophia Brilke, Lubna Dada, António Dias, Jonathan Duplissy, Imad El Haddad, Henning Finkenzeller, Lukas Fischer, Xucheng He, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Hanna E. Manninen, Ruby Marten, Bernhard Mentler, Eva Partoll, Tuukka Petäjä, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Mario Simon, Yee Jun Tham, Miguel Vazquez-Pufleau, Andrea C. Wagner, Yonghong Wang, Yusheng Wu, Mao Xiao, Urs Baltensperger, Joachim Curtius, Richard Flagan, Jasper Kirkby, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas Worsnop, and Neil M. Donahue. Environmental Science & Technology 2019 53 (21), 12357-12365. DOI: 10.1021/acs.est.9b03265
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:98865
Deposited By: Tony Diaz
Deposited On:25 Sep 2019 23:23
Last Modified:16 Nov 2021 17:42

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