TY - JOUR
T1 - Understanding Hygroscopic Nucleation of Sulfate Aerosols
T2 - Combination of Molecular Dynamics Simulation with Classical Nucleation Theory
AU - Zhao, Zheng
AU - Kong, Kewei
AU - Wang, Shixian
AU - Zhou, Yingcheng
AU - Cheng, Daojian
AU - Wang, Wenchuan
AU - Zeng, Xiao Cheng
AU - Li, Hui
N1 - Funding Information:
H.L. acknowledges funding support from National Natural Science Foundation of China (21773005). The computational resources utilized in this research were provided by Shanghai Supercomputer Center.
Publisher Copyright:
© 2019 American Chemical Society.
PY - 2019/3/7
Y1 - 2019/3/7
N2 - 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.
AB - 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.
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U2 - 10.1021/acs.jpclett.9b00152
DO - 10.1021/acs.jpclett.9b00152
M3 - Article
C2 - 30798591
AN - SCOPUS:85062520328
SN - 1948-7185
VL - 10
SP - 1126
EP - 1132
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 5
ER -