Arrhenius analysis of anisotropic surface self-diffusion on the prismatic facet of ice

Ivan Gladich, William Pfalzgraff, Ondřej Maršálek, Pavel Jungwirth, Martina Roeselová, Steven Neshyba

Research output: Contribution to journalArticle

17 Citations (Scopus)

Abstract

We present an Arrhenius analysis of self-diffusion on the prismatic surface of ice calculated from molecular dynamics simulations. The six-site water model of Nada and van der Eerden was used in combination with a structure-based criterion for determining the number of liquid-like molecules in the quasi-liquid layer. Simulated temperatures range from 230 K-287 K, the latter being just below the melting temperature of the model, 289 K. Calculated surface diffusion coefficients agree with available experimental data to within quoted precision. Our results indicate a positive Arrhenius curvature, implying a change in the mechanism of self-diffusion from low to high temperature, with a concomitant increase in energy of activation from 29.1 kJ mol-1 at low temperature to 53.8 kJ mol-1 close to the melting point. In addition, we find that the surface self-diffusion is anisotropic at lower temperatures, transitioning to isotropic in the temperature range of 240-250 K. We also present a framework for self-diffusion in the quasi-liquid layer on ice that aims to explain these observations.

Original languageEnglish
Pages (from-to)19960-19969
Number of pages10
JournalPhysical Chemistry Chemical Physics
Volume13
Issue number44
DOIs
Publication statusPublished - 28 Nov 2011
Externally publishedYes

Fingerprint

Ice
surface diffusion
flat surfaces
ice
Temperature
liquids
Melting point
Liquids
Freezing
Surface diffusion
melting points
temperature
diffusion coefficient
curvature
melting
activation
Molecular Dynamics Simulation
Molecular dynamics
molecular dynamics
Chemical activation

ASJC Scopus subject areas

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

Cite this

Gladich, I., Pfalzgraff, W., Maršálek, O., Jungwirth, P., Roeselová, M., & Neshyba, S. (2011). Arrhenius analysis of anisotropic surface self-diffusion on the prismatic facet of ice. Physical Chemistry Chemical Physics, 13(44), 19960-19969. https://doi.org/10.1039/c1cp22238d

Arrhenius analysis of anisotropic surface self-diffusion on the prismatic facet of ice. / Gladich, Ivan; Pfalzgraff, William; Maršálek, Ondřej; Jungwirth, Pavel; Roeselová, Martina; Neshyba, Steven.

In: Physical Chemistry Chemical Physics, Vol. 13, No. 44, 28.11.2011, p. 19960-19969.

Research output: Contribution to journalArticle

Gladich, I, Pfalzgraff, W, Maršálek, O, Jungwirth, P, Roeselová, M & Neshyba, S 2011, 'Arrhenius analysis of anisotropic surface self-diffusion on the prismatic facet of ice', Physical Chemistry Chemical Physics, vol. 13, no. 44, pp. 19960-19969. https://doi.org/10.1039/c1cp22238d
Gladich, Ivan ; Pfalzgraff, William ; Maršálek, Ondřej ; Jungwirth, Pavel ; Roeselová, Martina ; Neshyba, Steven. / Arrhenius analysis of anisotropic surface self-diffusion on the prismatic facet of ice. In: Physical Chemistry Chemical Physics. 2011 ; Vol. 13, No. 44. pp. 19960-19969.
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