Freezing point and solid-liquid interfacial free energy of stockmayer dipolar fluids: A molecular dynamics simulation study

Jun Wang, Pankaj A. Apte, James R. Morris, Xiao Cheng Zeng

Research output: Contribution to journalArticle

8 Citations (Scopus)

Abstract

Stockmayer fluids are a prototype model system for dipolar fluids. We have computed the freezing temperatures of Stockmayer fluids at zero pressure using three different molecular-dynamics simulation methods, namely, the superheating-undercooling method, the constant-pressure and constanttemperature two-phase coexistence method, and the constant-pressure and constant-enthalpy twophase coexistence method. The best estimate of the freezing temperature (in reduced unit) for the Stockmayer (SM) fluid with the dimensionless dipole moment μ *= 1, √ 2, √ 3 is 0.656 ± 0.001, 0.726 ± 0.002, and 0.835 ± 0.005, respectively. The freezing temperature increases with the dipolar strength. Moreover, for the first time, the solid-liquid interfacial free energies γ of the fcc (111), (110), and (100) interfaces are computed using two independent methods, namely, the cleavingwall method and the interfacial fluctuation method. Both methods predict that the interfacial free energy increases with the dipole moment. Although the interfacial fluctuation method suggests a weaker interfacial anisotropy, particularly for strongly dipolar SM fluids, both methods predicted the same trend of interfacial anisotropy, i.e., γ 100 > γ110 > γ111.

Original languageEnglish (US)
Article number114705
JournalJournal of Chemical Physics
Volume139
Issue number11
DOIs
StatePublished - Sep 21 2013

Fingerprint

Freezing
Free energy
melting points
Molecular dynamics
free energy
molecular dynamics
Fluids
fluids
freezing
Computer simulation
Liquids
liquids
Dipole moment
simulation
dipole moments
Anisotropy
superheating
anisotropy
Undercooling
supercooling

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Freezing point and solid-liquid interfacial free energy of stockmayer dipolar fluids : A molecular dynamics simulation study. / Wang, Jun; Apte, Pankaj A.; Morris, James R.; Zeng, Xiao Cheng.

In: Journal of Chemical Physics, Vol. 139, No. 11, 114705, 21.09.2013.

Research output: Contribution to journalArticle

@article{dcf2e12ccb4a4b8eafb3916c944e5357,
title = "Freezing point and solid-liquid interfacial free energy of stockmayer dipolar fluids: A molecular dynamics simulation study",
abstract = "Stockmayer fluids are a prototype model system for dipolar fluids. We have computed the freezing temperatures of Stockmayer fluids at zero pressure using three different molecular-dynamics simulation methods, namely, the superheating-undercooling method, the constant-pressure and constanttemperature two-phase coexistence method, and the constant-pressure and constant-enthalpy twophase coexistence method. The best estimate of the freezing temperature (in reduced unit) for the Stockmayer (SM) fluid with the dimensionless dipole moment μ *= 1, √ 2, √ 3 is 0.656 ± 0.001, 0.726 ± 0.002, and 0.835 ± 0.005, respectively. The freezing temperature increases with the dipolar strength. Moreover, for the first time, the solid-liquid interfacial free energies γ of the fcc (111), (110), and (100) interfaces are computed using two independent methods, namely, the cleavingwall method and the interfacial fluctuation method. Both methods predict that the interfacial free energy increases with the dipole moment. Although the interfacial fluctuation method suggests a weaker interfacial anisotropy, particularly for strongly dipolar SM fluids, both methods predicted the same trend of interfacial anisotropy, i.e., γ 100 > γ110 > γ111.",
author = "Jun Wang and Apte, {Pankaj A.} and Morris, {James R.} and Zeng, {Xiao Cheng}",
year = "2013",
month = "9",
day = "21",
doi = "10.1063/1.4821455",
language = "English (US)",
volume = "139",
journal = "Journal of Chemical Physics",
issn = "0021-9606",
publisher = "American Institute of Physics Publising LLC",
number = "11",

}

TY - JOUR

T1 - Freezing point and solid-liquid interfacial free energy of stockmayer dipolar fluids

T2 - A molecular dynamics simulation study

AU - Wang, Jun

AU - Apte, Pankaj A.

AU - Morris, James R.

AU - Zeng, Xiao Cheng

PY - 2013/9/21

Y1 - 2013/9/21

N2 - Stockmayer fluids are a prototype model system for dipolar fluids. We have computed the freezing temperatures of Stockmayer fluids at zero pressure using three different molecular-dynamics simulation methods, namely, the superheating-undercooling method, the constant-pressure and constanttemperature two-phase coexistence method, and the constant-pressure and constant-enthalpy twophase coexistence method. The best estimate of the freezing temperature (in reduced unit) for the Stockmayer (SM) fluid with the dimensionless dipole moment μ *= 1, √ 2, √ 3 is 0.656 ± 0.001, 0.726 ± 0.002, and 0.835 ± 0.005, respectively. The freezing temperature increases with the dipolar strength. Moreover, for the first time, the solid-liquid interfacial free energies γ of the fcc (111), (110), and (100) interfaces are computed using two independent methods, namely, the cleavingwall method and the interfacial fluctuation method. Both methods predict that the interfacial free energy increases with the dipole moment. Although the interfacial fluctuation method suggests a weaker interfacial anisotropy, particularly for strongly dipolar SM fluids, both methods predicted the same trend of interfacial anisotropy, i.e., γ 100 > γ110 > γ111.

AB - Stockmayer fluids are a prototype model system for dipolar fluids. We have computed the freezing temperatures of Stockmayer fluids at zero pressure using three different molecular-dynamics simulation methods, namely, the superheating-undercooling method, the constant-pressure and constanttemperature two-phase coexistence method, and the constant-pressure and constant-enthalpy twophase coexistence method. The best estimate of the freezing temperature (in reduced unit) for the Stockmayer (SM) fluid with the dimensionless dipole moment μ *= 1, √ 2, √ 3 is 0.656 ± 0.001, 0.726 ± 0.002, and 0.835 ± 0.005, respectively. The freezing temperature increases with the dipolar strength. Moreover, for the first time, the solid-liquid interfacial free energies γ of the fcc (111), (110), and (100) interfaces are computed using two independent methods, namely, the cleavingwall method and the interfacial fluctuation method. Both methods predict that the interfacial free energy increases with the dipole moment. Although the interfacial fluctuation method suggests a weaker interfacial anisotropy, particularly for strongly dipolar SM fluids, both methods predicted the same trend of interfacial anisotropy, i.e., γ 100 > γ110 > γ111.

UR - http://www.scopus.com/inward/record.url?scp=84903363763&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84903363763&partnerID=8YFLogxK

U2 - 10.1063/1.4821455

DO - 10.1063/1.4821455

M3 - Article

C2 - 24070303

AN - SCOPUS:84903363763

VL - 139

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

SN - 0021-9606

IS - 11

M1 - 114705

ER -