Understanding Hygroscopic Nucleation of Sulfate Aerosols: Combination of Molecular Dynamics Simulation with Classical Nucleation Theory

Zheng Zhao, Kewei Kong, Shixian Wang, Yingcheng Zhou, Daojian Cheng, Wenchuan Wang, Xiao Cheng Zeng, Hui Li

Research output: Contribution to journalArticle

Abstract

We present a combined molecular dynamics (MD) and classical nucleation theory (CNT) approach to address many issues regarding the nucleation of inorganic aerosols. By taking parameters from MD simulations, we find the CNT predicts fairly reasonable free-energy profiles for the hygroscopic nucleation of aerosols. Moreover, we find that the ionization of sulfates can play a key role in stabilizing aqueous clusters and that both the size of the critical nucleus and the nucleation barrier can be significantly lowered by the H 2 SO 4 and NH 4 HSO 4 , whereas the effect of NH 3 on nucleation is negligible. NH 4 HSO 4 provides stronger enhancement effect to aerosol formation than H 2 SO 4 . In view of the consistency between the theoretical prediction and experimental observation, the combination of MD simulation and CNT appears to be a valuable approach to gain deeper understanding of how aerosol nucleation is affected by different chemical species.

Original languageEnglish (US)
Pages (from-to)1126-1132
Number of pages7
JournalJournal of Physical Chemistry Letters
Volume10
Issue number5
DOIs
StatePublished - Mar 7 2019

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Aerosols
Sulfates
Molecular dynamics
sulfates
aerosols
Nucleation
nucleation
molecular dynamics
Computer simulation
simulation
Free energy
Ionization
free energy
ionization
nuclei
augmentation
profiles
predictions

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

Cite this

Understanding Hygroscopic Nucleation of Sulfate Aerosols : Combination of Molecular Dynamics Simulation with Classical Nucleation Theory. / Zhao, Zheng; Kong, Kewei; Wang, Shixian; Zhou, Yingcheng; Cheng, Daojian; Wang, Wenchuan; Zeng, Xiao Cheng; Li, Hui.

In: Journal of Physical Chemistry Letters, Vol. 10, No. 5, 07.03.2019, p. 1126-1132.

Research output: Contribution to journalArticle

Zhao, Zheng ; Kong, Kewei ; Wang, Shixian ; Zhou, Yingcheng ; Cheng, Daojian ; Wang, Wenchuan ; Zeng, Xiao Cheng ; Li, Hui. / Understanding Hygroscopic Nucleation of Sulfate Aerosols : Combination of Molecular Dynamics Simulation with Classical Nucleation Theory. In: Journal of Physical Chemistry Letters. 2019 ; Vol. 10, No. 5. pp. 1126-1132.
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