CERN Accelerating science

Article
Title	Molecular characterization of ultrafine particles using extractive electrospray time-of-flight mass spectrometry
Author(s)	Surdu, Mihnea (PSI, Villigen) ; Pospisilova, Veronika (PSI, Villigen) ; Xiao, Mao (PSI, Villigen) ; Wang, Mingyi (Carnegie Mellon U.) ; Mentler, Bernhard (Innsbruck U.) ; Simon, Mario (Frankfurt U., FIAS ; Frankfurt U.) ; Stolzenburg, Dominik (Vienna U., Dept. Math. ; Helsinki U.) ; Hoyle, Christopher R (PSI, Villigen ; Zurich, ETH) ; Bell, David M (PSI, Villigen) ; Lee, Chuan Ping (PSI, Villigen) ; Lamkaddam, Houssni (PSI, Villigen) ; Lopez-Hilfiker, Felipe (PSI, Villigen) ; Ahonen, Lauri R (Helsinki U.) ; Amorim, Antonio (Lisbon, CENTRA) ; Baccarini, Andrea (PSI, Villigen ; Ecole Polytechnique, Lausanne) ; Chen, Dexian (Carnegie Mellon U.) ; Dada, Lubna (PSI, Villigen ; Helsinki U.) ; Duplissy, Jonathan (Helsinki U. ; Helsinki Inst. of Phys.) ; Finkenzeller, Henning (Colorado U.) ; He, Xu-Cheng (Helsinki U.) ; Hofbauer, Victoria (Carnegie Mellon U.) ; Kim, Changhyuk (Caltech ; Pusan Natl. U.) ; Kürten, Andreas (Frankfurt U., FIAS ; Frankfurt U.) ; Kvashnin, Aleksandr (Lebedev Inst.) ; Lehtipalo, Katrianne (Helsinki U. ; Helsinki Inst. of Phys.) ; Makhmutov, Vladimir (Lebedev Inst.) ; Molteni, Ugo (PSI, Villigen) ; Nie, Wei (Nanjing U. (main)) ; Onnela, Antti (CERN) ; Petäjä, Tuukka (Helsinki U.) ; Quéléver, Lauriane L J (Helsinki U.) ; Tauber, Christian (Vienna U., Dept. Math.) ; Tomé, António (Beira Interior U., Covilha) ; Wagner, Robert (Helsinki U.) ; Yan, Chao (Helsinki U.) ; Prevot, Andre S H (PSI, Villigen) ; Dommen, Josef (PSI, Villigen) ; Donahue, Neil M (Carnegie Mellon U.) ; Hansel, Armin (Innsbruck U.) ; Curtius, Joachim (Frankfurt U., FIAS ; Frankfurt U.) ; Winkler, Paul M (Vienna U., Dept. Math.) ; Kulmala, Markku (Helsinki U. ; Helsinki Inst. of Phys.) ; Volkamer, Rainer (Colorado U.) ; Flagan, Richard C (Caltech) ; Kirkby, Jasper (Frankfurt U., FIAS ; Frankfurt U. ; CERN) ; Worsnop, Douglas R (Helsinki U. ; New England Nucl.) ; Slowik, Jay G (PSI, Villigen) ; Wang, Dongyu S (PSI, Villigen) ; Baltensperger, Urs (PSI, Villigen) ; el Haddad, Imad el (PSI, Villigen)
Publication	2021
Number of pages	15
In:	Environmental Science: Atmospheres 1 (2021) 434-448
DOI	10.1039/d1ea00050k
Subject category	Astrophysics and Astronomy
Accelerator/Facility, Experiment	CERN PS ; CLOUD
Abstract	Aerosol particles negatively affect human health while also having climatic relevance due to, for example, their ability to act as cloud condensation nuclei. Ultrafine particles (diameter D$_p$ < 100 nm) typically comprise the largest fraction of the total number concentration, however, their chemical characterization is difficult because of their low mass. Using an extractive electrospray time-of-flight mass spectrometer (EESI-TOF), we characterize the molecular composition of freshly nucleated particles from naphthalene and b-caryophyllene oxidation products at the CLOUD chamber at CERN. We perform a detailed intercomparison of the organic aerosol chemical composition measured by the EESI-TOF and an iodide adduct chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols (FIGAERO-I-CIMS). We also use an aerosol growth model based on the condensation of organic vapors to show that the chemical composition measured by the EESI-TOF is consistent with the expected condensed oxidation products. This agreement could be further improved by constraining the EESI-TOF compound-specific sensitivity or considering condensed-phase processes. Our results show that the EESI-TOF can obtain the chemical composition of particles as small as 20 nm in diameter with mass loadings as low as hundreds of ng m$^{-3}$ in real time. This was until now difficult to achieve, as other online instruments are often limited by size cutoffs, ionization/thermal fragmentation and/or semicontinuous sampling. Using real-time simultaneous gas- and particle-phase data, we discuss the condensation of naphthalene oxidation products on a molecular level.
Copyright/License	publication: (License: CC-BY-NC-3.0) © 2021-2024 The Author(s)

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