Molecular understanding of new-particle formation from <i>α</i>-pinene between −50 and +25&thinsp;°C

<p>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 &l...

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Main Authors: M. Simon, L. Dada, M. Heinritzi, W. Scholz, D. Stolzenburg, L. Fischer, A. C. Wagner, A. Kürten, B. Rörup, X.-C. He, J. Almeida, R. Baalbaki, A. Baccarini, P. S. Bauer, L. Beck, A. Bergen, F. Bianchi, S. Bräkling, S. Brilke, L. Caudillo, D. Chen, B. Chu, A. Dias, D. C. Draper, J. Duplissy, I. El-Haddad, H. Finkenzeller, C. Frege, L. Gonzalez-Carracedo, H. Gordon, M. Granzin, J. Hakala, V. Hofbauer, C. R. Hoyle, C. Kim, W. Kong, H. Lamkaddam, C. P. Lee, K. Lehtipalo, M. Leiminger, H. Mai, H. E. Manninen, G. Marie, R. Marten, B. Mentler, U. Molteni, L. Nichman, W. Nie, A. Ojdanic, A. Onnela, E. Partoll, T. Petäjä, J. Pfeifer, M. Philippov, L. L. J. Quéléver, A. Ranjithkumar, M. P. Rissanen, S. Schallhart, S. Schobesberger, S. Schuchmann, J. Shen, M. Sipilä, G. Steiner, Y. Stozhkov, C. Tauber, Y. J. Tham, A. R. Tomé, M. Vazquez-Pufleau, A. L. Vogel, R. Wagner, M. Wang, D. S. Wang, Y. Wang, S. K. Weber, Y. Wu, M. Xiao, C. Yan, P. Ye, Q. Ye, M. Zauner-Wieczorek, X. Zhou, U. Baltensperger, J. Dommen, R. C. Flagan, A. Hansel, M. Kulmala, R. Volkamer, P. M. Winkler, D. R. Worsnop, N. M. Donahue, J. Kirkby, J. Curtius
Format: Article
Language:English
Published: Copernicus Publications 2020-08-01
Series:Atmospheric Chemistry and Physics
Online Access:https://acp.copernicus.org/articles/20/9183/2020/acp-20-9183-2020.pdf
_version_ 1818300478987960320
author M. Simon
L. Dada
M. Heinritzi
W. Scholz
W. Scholz
D. Stolzenburg
L. Fischer
A. C. Wagner
A. C. Wagner
A. Kürten
B. Rörup
X.-C. He
J. Almeida
J. Almeida
R. Baalbaki
A. Baccarini
P. S. Bauer
L. Beck
A. Bergen
F. Bianchi
S. Bräkling
S. Brilke
L. Caudillo
D. Chen
B. Chu
A. Dias
A. Dias
D. C. Draper
J. Duplissy
J. Duplissy
I. El-Haddad
H. Finkenzeller
C. Frege
L. Gonzalez-Carracedo
H. Gordon
H. Gordon
M. Granzin
J. Hakala
V. Hofbauer
C. R. Hoyle
C. R. Hoyle
C. Kim
C. Kim
W. Kong
H. Lamkaddam
C. P. Lee
K. Lehtipalo
K. Lehtipalo
M. Leiminger
M. Leiminger
H. Mai
H. E. Manninen
G. Marie
R. Marten
B. Mentler
U. Molteni
L. Nichman
L. Nichman
W. Nie
A. Ojdanic
A. Onnela
E. Partoll
T. Petäjä
J. Pfeifer
J. Pfeifer
M. Philippov
L. L. J. Quéléver
A. Ranjithkumar
M. P. Rissanen
M. P. Rissanen
S. Schallhart
S. Schallhart
S. Schobesberger
S. Schuchmann
J. Shen
M. Sipilä
G. Steiner
G. Steiner
Y. Stozhkov
C. Tauber
Y. J. Tham
A. R. Tomé
M. Vazquez-Pufleau
A. L. Vogel
A. L. Vogel
R. Wagner
M. Wang
D. S. Wang
Y. Wang
S. K. Weber
Y. Wu
M. Xiao
C. Yan
P. Ye
P. Ye
Q. Ye
M. Zauner-Wieczorek
X. Zhou
X. Zhou
U. Baltensperger
J. Dommen
R. C. Flagan
A. Hansel
A. Hansel
M. Kulmala
M. Kulmala
M. Kulmala
M. Kulmala
R. Volkamer
P. M. Winkler
D. R. Worsnop
D. R. Worsnop
D. R. Worsnop
N. M. Donahue
J. Kirkby
J. Kirkby
J. Curtius
author_facet M. Simon
L. Dada
M. Heinritzi
W. Scholz
W. Scholz
D. Stolzenburg
L. Fischer
A. C. Wagner
A. C. Wagner
A. Kürten
B. Rörup
X.-C. He
J. Almeida
J. Almeida
R. Baalbaki
A. Baccarini
P. S. Bauer
L. Beck
A. Bergen
F. Bianchi
S. Bräkling
S. Brilke
L. Caudillo
D. Chen
B. Chu
A. Dias
A. Dias
D. C. Draper
J. Duplissy
J. Duplissy
I. El-Haddad
H. Finkenzeller
C. Frege
L. Gonzalez-Carracedo
H. Gordon
H. Gordon
M. Granzin
J. Hakala
V. Hofbauer
C. R. Hoyle
C. R. Hoyle
C. Kim
C. Kim
W. Kong
H. Lamkaddam
C. P. Lee
K. Lehtipalo
K. Lehtipalo
M. Leiminger
M. Leiminger
H. Mai
H. E. Manninen
G. Marie
R. Marten
B. Mentler
U. Molteni
L. Nichman
L. Nichman
W. Nie
A. Ojdanic
A. Onnela
E. Partoll
T. Petäjä
J. Pfeifer
J. Pfeifer
M. Philippov
L. L. J. Quéléver
A. Ranjithkumar
M. P. Rissanen
M. P. Rissanen
S. Schallhart
S. Schallhart
S. Schobesberger
S. Schuchmann
J. Shen
M. Sipilä
G. Steiner
G. Steiner
Y. Stozhkov
C. Tauber
Y. J. Tham
A. R. Tomé
M. Vazquez-Pufleau
A. L. Vogel
A. L. Vogel
R. Wagner
M. Wang
D. S. Wang
Y. Wang
S. K. Weber
Y. Wu
M. Xiao
C. Yan
P. Ye
P. Ye
Q. Ye
M. Zauner-Wieczorek
X. Zhou
X. Zhou
U. Baltensperger
J. Dommen
R. C. Flagan
A. Hansel
A. Hansel
M. Kulmala
M. Kulmala
M. Kulmala
M. Kulmala
R. Volkamer
P. M. Winkler
D. R. Worsnop
D. R. Worsnop
D. R. Worsnop
N. M. Donahue
J. Kirkby
J. Kirkby
J. Curtius
author_sort M. Simon
collection DOAJ
description <p>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 <span class="inline-formula"><i>α</i></span>-pinene, the most abundant monoterpene in the atmosphere. Due to their abundance and low volatility, HOMs can play an important role in 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 NPF 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 <span class="inline-formula">+25</span> to <span class="inline-formula">−50</span>&thinsp;<span class="inline-formula"><sup>∘</sup></span>C) results in a reduced HOM yield and reduced oxidation state of the products, whereas the NPF rates (<span class="inline-formula"><i>J</i><sub>1.7 nm</sub></span>) 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 two-dimensional volatility basis set (2D VBS) model provides their volatility distribution. The HOM yield decreases with temperature from 6.2&thinsp;% at 25&thinsp;<span class="inline-formula"><sup>∘</sup></span>C to 0.7&thinsp;% at <span class="inline-formula">−50</span>&thinsp;<span class="inline-formula"><sup>∘</sup></span>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 3 orders of magnitude at <span class="inline-formula">−50</span>&thinsp;<span class="inline-formula"><sup>∘</sup></span>C compared with 25&thinsp;<span class="inline-formula"><sup>∘</sup></span>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 NPF at the molecular level. Our measurements, therefore, improve our understanding of pure biogenic NPF for a wide range of tropospheric temperatures and precursor concentrations.</p>
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spelling doaj.art-cd6a89fdefa44cc2a7737d2c81b3b5212022-12-21T23:58:38ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242020-08-01209183920710.5194/acp-20-9183-2020Molecular understanding of new-particle formation from <i>α</i>-pinene between −50 and +25&thinsp;°CM. Simon0L. Dada1M. Heinritzi2W. Scholz3W. Scholz4D. Stolzenburg5L. Fischer6A. C. Wagner7A. C. Wagner8A. Kürten9B. Rörup10X.-C. He11J. Almeida12J. Almeida13R. Baalbaki14A. Baccarini15P. S. Bauer16L. Beck17A. Bergen18F. Bianchi19S. Bräkling20S. Brilke21L. Caudillo22D. Chen23B. Chu24A. Dias25A. Dias26D. C. Draper27J. Duplissy28J. Duplissy29I. El-Haddad30H. Finkenzeller31C. Frege32L. Gonzalez-Carracedo33H. Gordon34H. Gordon35M. Granzin36J. Hakala37V. Hofbauer38C. R. Hoyle39C. R. Hoyle40C. Kim41C. Kim42W. Kong43H. Lamkaddam44C. P. Lee45K. Lehtipalo46K. Lehtipalo47M. Leiminger48M. Leiminger49H. Mai50H. E. Manninen51G. Marie52R. Marten53B. Mentler54U. Molteni55L. Nichman56L. Nichman57W. Nie58A. Ojdanic59A. Onnela60E. Partoll61T. Petäjä62J. Pfeifer63J. Pfeifer64M. Philippov65L. L. J. Quéléver66A. Ranjithkumar67M. P. Rissanen68M. P. Rissanen69S. Schallhart70S. Schallhart71S. Schobesberger72S. Schuchmann73J. Shen74M. Sipilä75G. Steiner76G. Steiner77Y. Stozhkov78C. Tauber79Y. J. Tham80A. R. Tomé81M. Vazquez-Pufleau82A. L. Vogel83A. L. Vogel84R. Wagner85M. Wang86D. S. Wang87Y. Wang88S. K. Weber89Y. Wu90M. Xiao91C. Yan92P. Ye93P. Ye94Q. Ye95M. Zauner-Wieczorek96X. Zhou97X. Zhou98U. Baltensperger99J. Dommen100R. C. Flagan101A. Hansel102A. Hansel103M. Kulmala104M. Kulmala105M. Kulmala106M. Kulmala107R. Volkamer108P. M. Winkler109D. R. Worsnop110D. R. Worsnop111D. R. Worsnop112N. M. Donahue113J. Kirkby114J. Kirkby115J. Curtius116Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, GermanyInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandInstitute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, GermanyInstitute for Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, 6020, AustriaIonicon Analytik GmbH, Innsbruck, 6020, AustriaFaculty of Physics, University of Vienna, Vienna, 1090, AustriaInstitute for Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, 6020, AustriaInstitute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, GermanyDepartment of Chemistry & CIRES, University of Colorado Boulder, Boulder, CO 80309-0215, USAInstitute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, GermanyInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandCERN, Geneva, 1211, SwitzerlandFaculdade de Ciências, Universidade de Lisboa, Lisbon, 1749-016, PortugalInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI, Villigen, 5232, SwitzerlandFaculty of Physics, University of Vienna, Vienna, 1090, AustriaInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandInstitute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, GermanyInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandTOFWERK AG, Thun, 3600, SwitzerlandFaculty of Physics, University of Vienna, Vienna, 1090, AustriaInstitute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, GermanyCenter for Atmospheric Particle Studies, Carnegie Mellon University, 5000 Forbes Avenue, Pittsburgh, PA 15213, USAInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandCERN, Geneva, 1211, SwitzerlandFaculdade de Ciências, Universidade de Lisboa, Lisbon, 1749-016, PortugalDepartment of Chemistry, University of California, Irvine, CA 92697, USAInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandHelsinki Institute of Physics, University of Helsinki, Helsinki, 00014, FinlandLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI, Villigen, 5232, SwitzerlandDepartment of Chemistry & CIRES, University of Colorado Boulder, Boulder, CO 80309-0215, USALaboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI, Villigen, 5232, SwitzerlandFaculty of Physics, University of Vienna, Vienna, 1090, AustriaCenter for Atmospheric Particle Studies, Carnegie Mellon University, 5000 Forbes Avenue, Pittsburgh, PA 15213, USAHelsinki Institute of Physics, University of Helsinki, Helsinki, 00014, FinlandInstitute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, GermanyInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandCenter for Atmospheric Particle Studies, Carnegie Mellon University, 5000 Forbes Avenue, Pittsburgh, PA 15213, USALaboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI, Villigen, 5232, SwitzerlandInstitute for Atmospheric and Climate Science, Swiss Federal Institute of Technology, Zurich, 8092, SwitzerlandSchool of Civil and Environmental Engineering, Pusan National University, Busan, 46241, Republic of KoreaDivision of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USADivision of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USALaboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI, Villigen, 5232, SwitzerlandLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI, Villigen, 5232, SwitzerlandInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandFinnish Meteorological Institute, Helsinki, 00560, FinlandInstitute for Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, 6020, AustriaIonicon Analytik GmbH, Innsbruck, 6020, AustriaDivision of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USACERN, Geneva, 1211, SwitzerlandInstitute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, GermanyLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI, Villigen, 5232, SwitzerlandInstitute for Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, 6020, AustriaLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI, Villigen, 5232, SwitzerlandDepartment of Earth and Environmental Sciences, University of Manchester, Manchester, M13 9PL, UKpresent address: Aerospace Research Centre, National Research Council of Canada, Ottawa, ON, K1V 9B4, CanadaJoint International Research Laboratory of Atmospheric and Earth System Sciences, School of Atmospheric Sciences, Nanjing University, Nanjing, Jiangsu Province, ChinaFaculty of Physics, University of Vienna, Vienna, 1090, AustriaCERN, Geneva, 1211, SwitzerlandInstitute for Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, 6020, AustriaInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandInstitute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, GermanyCERN, Geneva, 1211, SwitzerlandP. N. Lebedev Physical Institute of the Russian Academy of Sciences, Moscow, 119991, RussiaInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandSchool of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UKInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandAerosol Physics Laboratory, Physics Unit, Faculty of Engineering and Natural Sciences, Tampere University, 33101 Tampere, FinlandInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandFinnish Meteorological Institute, Helsinki, 00560, FinlandDepartment of Applied Physics, University of Eastern Finland, Kuopio, 70211, FinlandCERN, Geneva, 1211, SwitzerlandInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandInstitute for Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, 6020, Austriapresent address: Grimm Aerosol Technik Ainring GmbH & Co KG, 83404 Ainring, GermanyP. N. Lebedev Physical Institute of the Russian Academy of Sciences, Moscow, 119991, RussiaFaculty of Physics, University of Vienna, Vienna, 1090, AustriaInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandIDL, Universidade da Beira Interior, R. Marquês de Ávila e Bolama, Covilhã, 6201-001, PortugalFaculty of Physics, University of Vienna, Vienna, 1090, AustriaInstitute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, GermanyCERN, Geneva, 1211, SwitzerlandInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandCenter for Atmospheric Particle Studies, Carnegie Mellon University, 5000 Forbes Avenue, Pittsburgh, PA 15213, USALaboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI, Villigen, 5232, SwitzerlandInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandCERN, Geneva, 1211, SwitzerlandInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandCERN, Geneva, 1211, SwitzerlandInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandCenter for Atmospheric Particle Studies, Carnegie Mellon University, 5000 Forbes Avenue, Pittsburgh, PA 15213, USAAerodyne Research Inc., Billerica, MA 01821, USACenter for Atmospheric Particle Studies, Carnegie Mellon University, 5000 Forbes Avenue, Pittsburgh, PA 15213, USAInstitute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, GermanyInstitute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, GermanyLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI, Villigen, 5232, SwitzerlandLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI, Villigen, 5232, SwitzerlandLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI, Villigen, 5232, SwitzerlandDivision of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USAInstitute for Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, 6020, AustriaIonicon Analytik GmbH, Innsbruck, 6020, AustriaInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandHelsinki Institute of Physics, University of Helsinki, Helsinki, 00014, FinlandJoint International Research Laboratory of Atmospheric and Earth System Sciences, School of Atmospheric Sciences, Nanjing University, Nanjing, Jiangsu Province, ChinaAerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, ChinaDepartment of Chemistry & CIRES, University of Colorado Boulder, Boulder, CO 80309-0215, USAFaculty of Physics, University of Vienna, Vienna, 1090, AustriaInstitute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, 00014, FinlandTOFWERK AG, Thun, 3600, SwitzerlandAerodyne Research Inc., Billerica, MA 01821, USACenter for Atmospheric Particle Studies, Carnegie Mellon University, 5000 Forbes Avenue, Pittsburgh, PA 15213, USAInstitute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, GermanyCERN, Geneva, 1211, SwitzerlandInstitute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany<p>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 <span class="inline-formula"><i>α</i></span>-pinene, the most abundant monoterpene in the atmosphere. Due to their abundance and low volatility, HOMs can play an important role in 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 NPF 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 <span class="inline-formula">+25</span> to <span class="inline-formula">−50</span>&thinsp;<span class="inline-formula"><sup>∘</sup></span>C) results in a reduced HOM yield and reduced oxidation state of the products, whereas the NPF rates (<span class="inline-formula"><i>J</i><sub>1.7 nm</sub></span>) 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 two-dimensional volatility basis set (2D VBS) model provides their volatility distribution. The HOM yield decreases with temperature from 6.2&thinsp;% at 25&thinsp;<span class="inline-formula"><sup>∘</sup></span>C to 0.7&thinsp;% at <span class="inline-formula">−50</span>&thinsp;<span class="inline-formula"><sup>∘</sup></span>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 3 orders of magnitude at <span class="inline-formula">−50</span>&thinsp;<span class="inline-formula"><sup>∘</sup></span>C compared with 25&thinsp;<span class="inline-formula"><sup>∘</sup></span>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 NPF at the molecular level. Our measurements, therefore, improve our understanding of pure biogenic NPF for a wide range of tropospheric temperatures and precursor concentrations.</p>https://acp.copernicus.org/articles/20/9183/2020/acp-20-9183-2020.pdf
spellingShingle M. Simon
L. Dada
M. Heinritzi
W. Scholz
W. Scholz
D. Stolzenburg
L. Fischer
A. C. Wagner
A. C. Wagner
A. Kürten
B. Rörup
X.-C. He
J. Almeida
J. Almeida
R. Baalbaki
A. Baccarini
P. S. Bauer
L. Beck
A. Bergen
F. Bianchi
S. Bräkling
S. Brilke
L. Caudillo
D. Chen
B. Chu
A. Dias
A. Dias
D. C. Draper
J. Duplissy
J. Duplissy
I. El-Haddad
H. Finkenzeller
C. Frege
L. Gonzalez-Carracedo
H. Gordon
H. Gordon
M. Granzin
J. Hakala
V. Hofbauer
C. R. Hoyle
C. R. Hoyle
C. Kim
C. Kim
W. Kong
H. Lamkaddam
C. P. Lee
K. Lehtipalo
K. Lehtipalo
M. Leiminger
M. Leiminger
H. Mai
H. E. Manninen
G. Marie
R. Marten
B. Mentler
U. Molteni
L. Nichman
L. Nichman
W. Nie
A. Ojdanic
A. Onnela
E. Partoll
T. Petäjä
J. Pfeifer
J. Pfeifer
M. Philippov
L. L. J. Quéléver
A. Ranjithkumar
M. P. Rissanen
M. P. Rissanen
S. Schallhart
S. Schallhart
S. Schobesberger
S. Schuchmann
J. Shen
M. Sipilä
G. Steiner
G. Steiner
Y. Stozhkov
C. Tauber
Y. J. Tham
A. R. Tomé
M. Vazquez-Pufleau
A. L. Vogel
A. L. Vogel
R. Wagner
M. Wang
D. S. Wang
Y. Wang
S. K. Weber
Y. Wu
M. Xiao
C. Yan
P. Ye
P. Ye
Q. Ye
M. Zauner-Wieczorek
X. Zhou
X. Zhou
U. Baltensperger
J. Dommen
R. C. Flagan
A. Hansel
A. Hansel
M. Kulmala
M. Kulmala
M. Kulmala
M. Kulmala
R. Volkamer
P. M. Winkler
D. R. Worsnop
D. R. Worsnop
D. R. Worsnop
N. M. Donahue
J. Kirkby
J. Kirkby
J. Curtius
Molecular understanding of new-particle formation from <i>α</i>-pinene between −50 and +25&thinsp;°C
Atmospheric Chemistry and Physics
title Molecular understanding of new-particle formation from <i>α</i>-pinene between −50 and +25&thinsp;°C
title_full Molecular understanding of new-particle formation from <i>α</i>-pinene between −50 and +25&thinsp;°C
title_fullStr Molecular understanding of new-particle formation from <i>α</i>-pinene between −50 and +25&thinsp;°C
title_full_unstemmed Molecular understanding of new-particle formation from <i>α</i>-pinene between −50 and +25&thinsp;°C
title_short Molecular understanding of new-particle formation from <i>α</i>-pinene between −50 and +25&thinsp;°C
title_sort molecular understanding of new particle formation from i α i pinene between 50 and 25 thinsp °c
url https://acp.copernicus.org/articles/20/9183/2020/acp-20-9183-2020.pdf
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