Density-Functional Tight-Binding Molecular Dynamics Simulations of Excess Proton Diffusion in Ice Ih, Ice Ic, Ice III, and Melted Ice VI Phases

研究成果: Article

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The structural, dynamical, and energetic properties of the excess proton in ice were studied using density-functional tight-binding molecular dynamics simulations. The ice systems investigated herein consisted of low-density hexagonal and cubic crystalline variants (ice Ih and Ic) and high-density structures (ice III and melted ice VI). Analysis of the temperature dependence of radial distribution function and bond order parameters served to characterize the distribution and configuration of hundreds of water molecules in a unit cell. We confirmed that ice Ih and Ic possess higher hexagonal symmetries than ice III and melted ice VI. The estimated Grotthuss shuttling diffusion coefficients in ice were larger than that of liquid water, indicating a slower proton diffusion process in high-density structures than in low-density systems. The energy barriers calculated on the basis of the Arrhenius plot of diffusion coefficients were in reasonable agreement with experimental measurement for ice Ih. Furthermore, the energy barriers for high-density structures were several times larger than those of low-density systems. The simulation results were likely related to the suppression of proton transfer in disordered water configurations, in particular, ice with low hexagonal symmetry.

元の言語English
ページ(範囲)33-40
ページ数8
ジャーナルJournal of Physical Chemistry A
122
発行部数1
DOI
出版物ステータスPublished - 2018 1 11

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Ice
Molecular dynamics
Protons
ice
molecular dynamics
protons
Computer simulation
simulation
Energy barriers
Water
diffusion coefficient
water
Arrhenius plots
Proton transfer
symmetry
configurations
radial distribution
Distribution functions
plots
distribution functions

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

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title = "Density-Functional Tight-Binding Molecular Dynamics Simulations of Excess Proton Diffusion in Ice Ih, Ice Ic, Ice III, and Melted Ice VI Phases",
abstract = "The structural, dynamical, and energetic properties of the excess proton in ice were studied using density-functional tight-binding molecular dynamics simulations. The ice systems investigated herein consisted of low-density hexagonal and cubic crystalline variants (ice Ih and Ic) and high-density structures (ice III and melted ice VI). Analysis of the temperature dependence of radial distribution function and bond order parameters served to characterize the distribution and configuration of hundreds of water molecules in a unit cell. We confirmed that ice Ih and Ic possess higher hexagonal symmetries than ice III and melted ice VI. The estimated Grotthuss shuttling diffusion coefficients in ice were larger than that of liquid water, indicating a slower proton diffusion process in high-density structures than in low-density systems. The energy barriers calculated on the basis of the Arrhenius plot of diffusion coefficients were in reasonable agreement with experimental measurement for ice Ih. Furthermore, the energy barriers for high-density structures were several times larger than those of low-density systems. The simulation results were likely related to the suppression of proton transfer in disordered water configurations, in particular, ice with low hexagonal symmetry.",
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AU - Sakti, Aditya Wibawa

AU - Nishimura, Yoshifumi

AU - Chou, Chien Pin

AU - Nakai, Hiromi

PY - 2018/1/11

Y1 - 2018/1/11

N2 - The structural, dynamical, and energetic properties of the excess proton in ice were studied using density-functional tight-binding molecular dynamics simulations. The ice systems investigated herein consisted of low-density hexagonal and cubic crystalline variants (ice Ih and Ic) and high-density structures (ice III and melted ice VI). Analysis of the temperature dependence of radial distribution function and bond order parameters served to characterize the distribution and configuration of hundreds of water molecules in a unit cell. We confirmed that ice Ih and Ic possess higher hexagonal symmetries than ice III and melted ice VI. The estimated Grotthuss shuttling diffusion coefficients in ice were larger than that of liquid water, indicating a slower proton diffusion process in high-density structures than in low-density systems. The energy barriers calculated on the basis of the Arrhenius plot of diffusion coefficients were in reasonable agreement with experimental measurement for ice Ih. Furthermore, the energy barriers for high-density structures were several times larger than those of low-density systems. The simulation results were likely related to the suppression of proton transfer in disordered water configurations, in particular, ice with low hexagonal symmetry.

AB - The structural, dynamical, and energetic properties of the excess proton in ice were studied using density-functional tight-binding molecular dynamics simulations. The ice systems investigated herein consisted of low-density hexagonal and cubic crystalline variants (ice Ih and Ic) and high-density structures (ice III and melted ice VI). Analysis of the temperature dependence of radial distribution function and bond order parameters served to characterize the distribution and configuration of hundreds of water molecules in a unit cell. We confirmed that ice Ih and Ic possess higher hexagonal symmetries than ice III and melted ice VI. The estimated Grotthuss shuttling diffusion coefficients in ice were larger than that of liquid water, indicating a slower proton diffusion process in high-density structures than in low-density systems. The energy barriers calculated on the basis of the Arrhenius plot of diffusion coefficients were in reasonable agreement with experimental measurement for ice Ih. Furthermore, the energy barriers for high-density structures were several times larger than those of low-density systems. The simulation results were likely related to the suppression of proton transfer in disordered water configurations, in particular, ice with low hexagonal symmetry.

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