Molecular understanding of new-particle formation from alpha-pinene between −50 °C and 25 °C Article Swipe
Mario Simon
,
Lubna Dada
,
Martin Heinritzi
,
Wiebke Scholz
,
Dominik Stolzenburg
,
Lukas Fischer
,
Andrea C. Wagner
,
Andreas Kürten
,
Birte Rörup
,
Xu‐Cheng He
,
João Paulo A. Almeida
,
Rima Baalbaki
,
Andrea Baccarini
,
Paulus S. Bauer
,
Lisa Beck
,
Anton Bergen
,
Federico Bianchi
,
Steffen Bräkling
,
Sophia Brilke
,
Lucía Caudillo
,
Dexian Chen
,
Biwu Chu
,
António Dias
,
Danielle C. Draper
,
Jonathan Duplissy
,
Imad El Haddad
,
Henning Finkenzeller
,
Carla Frege
,
Loïc Gonzalez-Carracedo
,
Hamish Gordon
,
Manuel Granzin
,
Jani Hakala
,
Victoria Hofbauer
,
C. R. Hoyle
,
Changhyuk Kim
,
Weimeng Kong
,
Houssni Lamkaddam
,
Chuan Ping Lee
,
Katrianne Lehtipalo
,
Markus Leiminger
,
Huajun Mai
,
Hanna E. Manninen
,
Guillaume Marie
,
Ruby Marten
,
Bernhard Mentler
,
Ugo Molteni
,
Leonid Nichman
,
Wei Nie
,
Andrea Ojdanic
,
Antti Onnela
,
Eva Partoll
,
Tuukka Petäjä
,
Joschka Pfeifer
,
Maxim Philippov
,
Lauriane L. J. Quéléver
,
Ananth Ranjithkumar
,
Matti Rissanen
,
Simon Schallhart
,
Siegfried Schobesberger
,
Simone Schuchmann
,
Jiali Shen
,
Mikko Sipilä
,
Gerhard Steiner
,
Y. I. Stozhkov
,
Christian Tauber
,
Yee Jun Tham
,
António Tomé
,
Miguel Vazquez‐Pufleau
,
Alexander L. Vogel
,
Robert Wagner
,
Mingyi Wang
,
Dongyu Wang
,
Yonghong Wang
,
Stefan K. Weber
,
Y. Wu
,
Mao Xiao
,
Chao Yan
,
Penglin Ye
,
Qing Ye
,
Marcel Zauner-Wieczorek
,
Xueqin Zhou
,
Urs Baltensperger
,
Josef Dommen
,
Rick C. Flagan
,
Armin Hansel
,
Markku Kulmala
,
Rainer Volkamer
,
Paul M. Winkler
,
Douglas R. Worsnop
,
Neil M. Donahue
,
J. Kirkby
,
Joachim Curtius
·
YOU?
·
· 2020
· Open Access
·
· DOI: https://doi.org/10.5194/acp-2019-1058
YOU?
·
· 2020
· Open Access
·
· DOI: https://doi.org/10.5194/acp-2019-1058
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.
Related Topics
Concepts
Chemistry
Aerosol
Volatility (finance)
Autoxidation
Chemical ionization
Atmospheric-pressure chemical ionization
Photochemistry
Analytical Chemistry (journal)
Ionization
Organic chemistry
Ion
Financial economics
Economics
Metadata
- Type
- preprint
- Language
- en
- Landing Page
- https://doi.org/10.5194/acp-2019-1058
- https://doi.org/10.5194/acp-2019-1058
- OA Status
- gold
- Cited By
- 8
- References
- 70
- Related Works
- 10
- OpenAlex ID
- https://openalex.org/W4238236304
All OpenAlex metadata
Raw OpenAlex JSON
- OpenAlex ID
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https://openalex.org/W4238236304Canonical identifier for this work in OpenAlex
- DOI
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https://doi.org/10.5194/acp-2019-1058Digital Object Identifier
- Title
-
Molecular understanding of new-particle formation from alpha-pinene between −50 °C and 25 °CWork title
- Type
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preprintOpenAlex work type
- Language
-
enPrimary language
- Publication year
-
2020Year of publication
- Publication date
-
2020-01-21Full publication date if available
- Authors
-
Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu‐Cheng He, João Paulo A. Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucía Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El Haddad, Henning Finkenzeller, Carla Frege, Loïc Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, C. R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Y. I. Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez‐Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu Wang, Yonghong Wang, Stefan K. Weber, Y. Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Rick C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, J. Kirkby, Joachim CurtiusList of authors in order
- Landing page
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https://doi.org/10.5194/acp-2019-1058Publisher landing page
- PDF URL
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https://doi.org/10.5194/acp-2019-1058Direct link to full text PDF
- Open access
-
YesWhether a free full text is available
- OA status
-
goldOpen access status per OpenAlex
- OA URL
-
https://doi.org/10.5194/acp-2019-1058Direct OA link when available
- Concepts
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Chemistry, Aerosol, Volatility (finance), Autoxidation, Chemical ionization, Atmospheric-pressure chemical ionization, Photochemistry, Analytical Chemistry (journal), Ionization, Organic chemistry, Ion, Financial economics, EconomicsTop concepts (fields/topics) attached by OpenAlex
- Cited by
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8Total citation count in OpenAlex
- Citations by year (recent)
-
2023: 1, 2022: 1, 2020: 6Per-year citation counts (last 5 years)
- References (count)
-
70Number of works referenced by this work
- Related works (count)
-
10Other works algorithmically related by OpenAlex
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