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Role of gas–molecular cluster–aerosol dynamics in atmospheric new-particle formation

Olenius, Tinja and Roldin, Pontus LU (2022) In Scientific Reports 12(1).
Abstract

New-particle formation from vapors through molecular cluster formation is a central process affecting atmospheric aerosol and cloud condensation nuclei numbers, and a significant source of uncertainty in assessments of aerosol radiative forcing. While advances in experimental and computational methods provide improved assessments of particle formation rates from different species, the standard approach to implement these data in aerosol models rests on highly simplifying assumptions concerning gas–cluster–aerosol dynamics. To quantify the effects of the simplifications, we develop an open-source tool for explicitly simulating the dynamics of the complete particle size spectrum from vapor molecules and molecular clusters to larger... (More)

New-particle formation from vapors through molecular cluster formation is a central process affecting atmospheric aerosol and cloud condensation nuclei numbers, and a significant source of uncertainty in assessments of aerosol radiative forcing. While advances in experimental and computational methods provide improved assessments of particle formation rates from different species, the standard approach to implement these data in aerosol models rests on highly simplifying assumptions concerning gas–cluster–aerosol dynamics. To quantify the effects of the simplifications, we develop an open-source tool for explicitly simulating the dynamics of the complete particle size spectrum from vapor molecules and molecular clusters to larger aerosols for multi-compound new-particle formation. We demonstrate that the simplified treatment is a reasonable approximation for particle formation from weakly clustering chemical compounds, but results in overprediction of particle numbers and of the contribution of new-particle formation to cloud condensation nuclei for strongly clustering, low-concentration trace gases. The new explicit approach circumvents these issues, thus enabling robust model–measurement comparisons, improved assessment of the importance of different particle formation agents, and construction of optimal simplifications for large-scale models.

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author
and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Scientific Reports
volume
12
issue
1
article number
10135
publisher
Nature Publishing Group
external identifiers
  • pmid:35710742
  • scopus:85132082045
ISSN
2045-2322
DOI
10.1038/s41598-022-14525-y
project
Continental Biosphere Aerosol Cloud climate feedback loop during the Anthropocene
Modelling atmospheric new particle formation from first principles – The role of Highly Oxygenated organic Molecules in clean and polluted air
language
English
LU publication?
yes
id
6c804627-f925-4aa3-9430-93110f352059
date added to LUP
2022-08-26 14:28:32
date last changed
2024-06-13 07:59:40
@article{6c804627-f925-4aa3-9430-93110f352059,
  abstract     = {{<p>New-particle formation from vapors through molecular cluster formation is a central process affecting atmospheric aerosol and cloud condensation nuclei numbers, and a significant source of uncertainty in assessments of aerosol radiative forcing. While advances in experimental and computational methods provide improved assessments of particle formation rates from different species, the standard approach to implement these data in aerosol models rests on highly simplifying assumptions concerning gas–cluster–aerosol dynamics. To quantify the effects of the simplifications, we develop an open-source tool for explicitly simulating the dynamics of the complete particle size spectrum from vapor molecules and molecular clusters to larger aerosols for multi-compound new-particle formation. We demonstrate that the simplified treatment is a reasonable approximation for particle formation from weakly clustering chemical compounds, but results in overprediction of particle numbers and of the contribution of new-particle formation to cloud condensation nuclei for strongly clustering, low-concentration trace gases. The new explicit approach circumvents these issues, thus enabling robust model–measurement comparisons, improved assessment of the importance of different particle formation agents, and construction of optimal simplifications for large-scale models.</p>}},
  author       = {{Olenius, Tinja and Roldin, Pontus}},
  issn         = {{2045-2322}},
  language     = {{eng}},
  number       = {{1}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Scientific Reports}},
  title        = {{Role of gas–molecular cluster–aerosol dynamics in atmospheric new-particle formation}},
  url          = {{http://dx.doi.org/10.1038/s41598-022-14525-y}},
  doi          = {{10.1038/s41598-022-14525-y}},
  volume       = {{12}},
  year         = {{2022}},
}