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© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 21 Jan 2020

Submitted as: research article | 21 Jan 2020

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A revised version of this preprint is currently under review for the journal ACP.

Molecular understanding of new-particle formation from alpha-pinene between −50 °C and 25 °C

Mario Simon1, Lubna Dada2, Martin Heinritzi1, Wiebke Scholz3,4, Dominik Stolzenburg5, Lukas Fischer3, Andrea C. Wagner1,6, Andreas Kürten1, Birte Rörup2, Xu-Cheng He2, João Almeida7,8, Rima Baalbaki2, Andrea Baccarini9, Paulus S. Bauer5, Lisa Beck2, Anton Bergen1, Federico Bianchi2, Steffen Bräkling10, Sophia Brilke5, Lucia Caudillo1, Dexian Chen11, Biwu Chu2, António Dias7,8, Danielle C. Draper12, Jonathan Duplissy2,13, Imad El Haddad9, Henning Finkenzeller6, Carla Frege9, Loic Gonzalez-Carracedo5, Hamish Gordon11,13, Manuel Granzin1, Jani Hakala2, Victoria Hofbauer11, Christopher R. Hoyle9,15, Changhyuk Kim16,17, Weimeng Kong17, Houssni Lamkaddam9, Chuan P. Lee9, Katrianne Lehtipalo2,18, Markus Leiminger3,4, Huajun Mai17, Hanna E. Manninen7, Guillaume Marie1, Ruby Marten9, Bernhard Mentler3, Ugo Molteni9, Leonid Nichman19,a, Wei Nie20, Andrea Ojdanic5, Antti Onnela7, Eva Partoll3, Tuukka Petäjä2, Joschka Pfeifer1,7, Maxim Philippov21, Lauriane L. J. Quéléver2, Ananth Ranjithkumar14, Matti Rissanen2,22, Simon Schallhart2,18, Siegfried Schobesberger23, Simone Schuchmann7, Jiali Shen2, Mikko Sipilä2, Gerhard Steiner3,b, Yuri Stozhkov21, Christian Tauber5, Yee J. Tham2, António R. Tomé24, Miguel Vazquez-Pufleau5, Alexander Vogel1,7, Robert Wagner2, Mingyi Wang11, Dongyu S. Wang9, Yonghong Wang2, Stefan K. Weber7, Yusheng Wu2, Mao Xiao7, Chao Yan2, Penglin Ye11,25, Qing Ye11, Marcel Zauner-Wieczorek1, Xueqin Zhou1,9, Urs Baltensperger9, Josef Dommen9, Rick C. Flagan17, Armin Hansel3,4, Markku Kulmala2,13,20,26, Rainer Volkamer6, Paul M. Winkler5, Douglas R. Worsnop2,10,25, Neil M. Donahue11, Jasper Kirkby1,7, and Joachim Curtius1 Mario Simon et al.
  • 1Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt am Main, 60438, Germany
  • 2Institute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, Finland
  • 3Institute for Ion and Applied Physics, University of Innsbruck, Innsbruck, 6020, Austria
  • 4Ionicon Analytik, Ges.m.b.H., Innsbruck, 6020, Austria
  • 5Faculty of Physics, University of Vienna, Vienna, 1090, Austria
  • 6Department of Chemistry & CIRES, University of Colorado Boulder, Boulder, CO, 80309-0215, USA
  • 7CERN, Geneva, 1211, Switzerland
  • 8Faculdade de Ciências, Universidade de Lisboa, Lisboa, 1749-016, Portugal
  • 9Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI, Villigen, 5232, Switzerland
  • 10TOFWERK AG, Thun, 3600, Switzerland
  • 11Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA, USA
  • 12Department of Chemistry, University of California, Irvine, CA, 92697, USA
  • 13Helsinki Institute of Physics, University of Helsinki, Helsinki, 00014, Finland
  • 14School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK
  • 15Institute for Atmospheric and Climate Science, Swiss Federal Institute of Technology, Zurich, 8092, Switzerland
  • 16School of Civil and Environmental Engineering, Pusan National University, Busan, 46241, Republic of Korea
  • 17Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA, 91125, USA
  • 18Finnish Meteorological Institute, Helsinki, 00560, Finland
  • 19School of Earth and Environmental Sciences, University of Manchester, Manchester, M13 9PL, UK
  • 20Joint International Research Laboratory of Atmospheric and Earth System Sciences, School of Atmospheric Sciences, Nanjing University, Nanjing, Jiangsu Province, China
  • 21P. N. Lebedev Physical Institute of the Russian Academy of Sciences, Moscow, 119991, Russia
  • 22Aerosol Physics Laboratory, Physics Unit, Faculty of Engineering and Natural Sciences, Tampere University, Tampere, Finland
  • 23Department of Applied Physics, University of Eastern Finland, Kuopio, 70211, Finland
  • 24IDL – Universidade da Beira Interior, R. Marquês de Ávila e Bolama, Covilhã, 6201-001, Portugal
  • 25Aerodyne Research Inc., Billerica, MA, 01821, USA
  • 26Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China
  • apresent address: Flight Research Laboratory, National Research Council of Canada, Ottawa, ON, K1V 9B4, Canada
  • bpresent address: Grimm Aerosol Technik Ainring GmbH & Co KG, Ainring, 83404, Germany

Abstract. Highly-oxygenated organic molecules (HOMs) contribute substantially to the formation and growth of atmospheric aerosol particles, which affect air quality, human health and Earth's climate. HOMs are formed by rapid, gas-phase autoxidation of volatile organic compounds (VOCs) such as α-pinene, the most abundant monoterpene in the atmosphere. Due to their abundance and low volatility, HOMs can play an important role for new-particle formation (NPF) and the early growth of atmospheric aerosols, even without any further assistance of other low-volatility compounds such as sulfuric acid. Both the autoxidation reaction forming HOMs and their new-particle formation rates are expected to be strongly dependent on temperature. However, experimental data on both effects are limited. Dedicated experiments were performed at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN to address this question. In this study, we show that a decrease in temperature (from +25 to −50 °C) results in a reduced HOM yield and reduced oxidation state of the products, whereas the new-particle formation rates (J1.7 nm) increase substantially. Measurements with two different chemical ionization mass spectrometers (using nitrate and protonated water as reagent ion, respectively) provide the molecular composition of the gaseous oxidation products and a 2-dimensional volatility basis set model (2D-VBS) provides their volatility distribution. The HOM yield decreases with temperature from 6.2 % at 25 °C to 0.7 % at −50 °C. However, there is a strong reduction of the saturation vapor pressure of each oxidation state as the temperature is reduced. Overall, the reduction in volatility with temperature leads to an increase in the nucleation rates by up to three orders of magnitude at −50 °C compared with 25 °C. In addition, the enhancement of the nucleation rates by ions decreases with decreasing temperature, since the neutral molecular clusters have increased stability against evaporation. The resulting data quantify how the interplay between the temperature-dependent oxidation pathways and the associated vapor pressures affect biogenic new-particle formation at the molecular level. Our measurements therefore improve our understanding of pure biogenic new-particle formation for a wide range of tropospheric temperatures and precursor concentrations.

Mario Simon et al.

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Mario Simon et al.

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Short summary
Highly-oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide range of tropospheric temperatures. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
Highly-oxygenated organic compounds (HOMs) have been identified as key vapors involved in...