TY - JOUR
T1 - Extended study of molecular dynamics simulation of homogeneous vapor-liquid nucleation of water
AU - Matsubara, Hiroki
AU - Koishi, Takahiro
AU - Ebisuzaki, Toshikazu
AU - Yasuoka, Kenji
N1 - Funding Information:
H.M. is supported by the Special Coordination Fund for Promoting Science and Technology (GRAPE-DR project), Ministry of Education, Culture, Sports, Science and Technology, Japan.
PY - 2007
Y1 - 2007
N2 - Using the simple point charge/extended water model, we performed molecular dynamics simulations of homogeneous vapor-liquid nucleation at various values of temperature T and supersaturation S, from which the nucleation rate J, critical nucleus size n*, and the cluster formation free energy ΔG were derived. As well as providing lots of simulation data, the results were compared with theories on homogeneous nucleation, including the classical, semiphenomenological, and scaled models, but none of these gave a satisfactory explanation for our results. It was found that two main factors made the theories fail: (1) The average cluster structure including the nonspherical shape and the core structure that is not like the bulk liquid and (2) the forward rate which is larger than assumed by the theories by about one order of magnitude. The quantitative evaluation of these factors is left for future investigations.
AB - Using the simple point charge/extended water model, we performed molecular dynamics simulations of homogeneous vapor-liquid nucleation at various values of temperature T and supersaturation S, from which the nucleation rate J, critical nucleus size n*, and the cluster formation free energy ΔG were derived. As well as providing lots of simulation data, the results were compared with theories on homogeneous nucleation, including the classical, semiphenomenological, and scaled models, but none of these gave a satisfactory explanation for our results. It was found that two main factors made the theories fail: (1) The average cluster structure including the nonspherical shape and the core structure that is not like the bulk liquid and (2) the forward rate which is larger than assumed by the theories by about one order of magnitude. The quantitative evaluation of these factors is left for future investigations.
UR - http://www.scopus.com/inward/record.url?scp=36849006353&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=36849006353&partnerID=8YFLogxK
U2 - 10.1063/1.2803899
DO - 10.1063/1.2803899
M3 - Article
AN - SCOPUS:36849006353
SN - 0021-9606
VL - 127
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 21
M1 - 214507
ER -