Preprints
https://doi.org/10.5194/acp-2021-512
https://doi.org/10.5194/acp-2021-512

  07 Jul 2021

07 Jul 2021

Review status: a revised version of this preprint was accepted for the journal ACP.

Chemical composition of nanoparticles from α-pinene nucleation and the influence of isoprene and relative humidity at low temperature

Lucía Caudillo1, Birte Rörup2, Martin Heinritzi1, Guillaume Marie1, Mario Simon1, Andrea C. Wagner3, Tatjana Müller1,4, Manuel Granzin1, Antonio Amorim5, Farnoush Ataei6, Rima Baalbaki2, Barbara Bertozzi7, Zoé Brasseur2, Randall Chiu3, Biwu Chu2, Lubna Dada8, Jonathan Duplissy2,9, Henning Finkenzeller3, Loïc Gonzalez Carracedo10, Xu-Cheng He2, Victoria Hofbauer11, Weimeng Kong12,13, Houssni Lamkaddam8, Chuan P. Lee8, Brandon Lopez11, Naser G. A. Mahfouz11, Vladimir Makhmutov14,26, Hanna E. Manninen15, Ruby Marten8, Dario Massabò16, Roy L. Mauldin17,11, Bernhard Mentler18, Ugo Molteni8,20,21, Antti Onnela15, Joschka Pfeifer15, Maxim Philippov14, Ana A. Piedehierro22, Meredith Schervish11, Wiebke Scholz18, Benjamin Schulze12, Jiali Shen2, Dominik Stolzenburg2, Yuri Stozhkov14, Mihnea Surdu8, Christian Tauber10, Yee Jun Tham2, Ping Tian23, António Tomé24, Steffen Vogt7, Mingyi Wang11, Dongyu S. Wang8, Stefan K. Weber15, André Welti22, Wang Yonghong2, Wu Yusheng2, Marcel Zauner-Wieczorek1, Urs Baltensperger8, Imad El Haddad8, Richard C. Flagan12, Armin Hansel18,19, Kristina Höhler7, Jasper Kirkby1,15, Markku Kulmala2,9,25, Katrianne Lehtipalo2,22, Ottmar Möhler7, Harald Saathoff7, Rainer Volkamer3, Paul M. Winkler10, Neil M. Donahue11, Andreas Kürten1, and Joachim Curtius1 Lucía Caudillo et al.
  • 1Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
  • 2Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
  • 3Department of Chemistry & CIRES, University of Colorado Boulder, Boulder, CO, 80309-0215, USA
  • 4Max Planck Institute for Chemistry, Mainz, 55128, Germany
  • 5CENTRA and FCUL, University of Lisbon, 1749-016 Lisbon, Portugal
  • 6Leibniz Institute for Tropospheric Research, Leipzig, 04318, Germany
  • 7Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein-Leopoldshafen, Germany
  • 8Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
  • 9Helsinki Institute of Physics, University of Helsinki, 00014 Helsinki, Finland
  • 10Faculty of Physics, University of Vienna, 1090 Vienna, Austria
  • 11Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA, 15213, USA
  • 12Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USA
  • 13California Air Resources Board, Sacramento, CA 95814, USA
  • 14Lebedev Physical Institute, Russian Academy of Sciences, 119991, Moscow, Russia
  • 15CERN, 1211 Geneva, Switzerland
  • 16Dipartimento di Fisica, Università di Genova and INFN, 16146 Genova, Italy
  • 17Department of Atmospheric and Oceanic Sciences, University of Colorado Boulder, Boulder, CO 80309, USA
  • 18Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
  • 19Ionicon Analytik GmbH, 6020 Innsbruck, Austria
  • 20Forest Dynamics, Swiss Federal Institute for Forest, Snow and Landscape Research, 8903 Birmensdorf, Switzerland
  • 21Department of Chemistry, University of California, Irvine, Irvine, CA 92697, USA
  • 22Finnish Meteorological Institute, 00560 Helsinki, Finland
  • 23Beijing Weather Modification Office, China
  • 24IDL, Universidade da Beira Interior, R. Marquês de Ávila e Bolama, Covilhã, 6201-001, Portugal
  • 25Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, P.R. China
  • 26Moscow Institute of Physics and Technology (National Research University), 117303, Moscow, Russia

Abstract. New Particle Formation (NPF) from biogenic organic precursors is an important atmospheric process. One of the major species is α-pinene, which upon oxidation, can form a suite of products covering a wide range of volatilities. A fraction of the oxidation products is termed Highly Oxygenated Organic Molecules (HOM). These play a crucial role for nucleation and the formation of Secondary Organic Aerosol (SOA). However, measuring the composition of newly formed particles is challenging due to their very small mass. Here, we present results on the gas and particle phase chemical composition for a system where α-pinene was oxidized by ozone, and for a mixed system of α-pinene and isoprene, respectively. The measurements took place at the CERN Cosmics Leaving Outdoor Droplets (CLOUD) chamber at temperatures between −50 °C and −30 °C and at low and high relative humidity (20 % and 60 to 100 % RH). These conditions were chosen to simulate pure biogenic new particle formation in the upper free troposphere. The particle chemical composition was analyzed by the Thermal Desorption-Differential Mobility Analyzer (TD-DMA) coupled to a nitrate chemical ionization time-of-flight mass spectrometer. This instrument can be used for particle and gas phase measurements using the same ionization and detection scheme. Our measurements revealed the presence of C8-10 monomers and C18-20 dimers as the major compounds in the particles (diameter up to ~ 100 nm). Particularly, for the system with isoprene added, C5 (C5H10O5-7) and C15 compounds (C15H24O5-10) are detected. This observation is consistent with the previously observed formation of such compounds in the gas phase. However, although the C5 and C15 compounds do not easily nucleate, our measurements indicate that they can still contribute to the particle growth at free tropospheric conditions. For the experiments reported here, most likely isoprene might enhance growth at particle sizes larger than 15 nm. Besides the chemical information regarding the HOM formation for the α-pinene (plus isoprene) system, we report on the nucleation rates measured at 1.7 nm and found that the lower J1.7nm values compared with previous studies are very likely due to the higher α-pinene and ozone mixing ratios used in the present study

Lucía Caudillo et al.

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-512', Anonymous Referee #1, 28 Jul 2021
  • RC2: 'Review of Caudillo et al.', Anonymous Referee #2, 11 Aug 2021

Lucía Caudillo et al.

Lucía Caudillo et al.

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Short summary
We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 °C and −50 °C). We measured particle and gas phase and found that most of the compounds that are present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8-10 and C18-20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 °C, 20 % RH.
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