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Journal of Chemical Physics / Volume 135 / Issue 24 / ARTICLES / Condensed Phase Dynamics, Structure, and Thermodynamics: Spectroscopy, Reactions, and Relaxation

J. Chem. Phys. 135, 244511 (2011); http://dx.doi.org/10.1063/1.3671993 (9 pages)

Energy relaxation of intermolecular motions in supercooled water and ice: A molecular dynamics study

Takuma Yagasaki1 and Shinji Saito1,2

1Department of Theoretical and Computational Molecular Science, Institute for Molecular Science, Myodaiji, Okazaki, Aichi, 444-8585, Japan
2The Graduate University for Advanced Studies, Myodaiji, Okazaki, Aichi, 444-8585, Japan

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(Received 19 October 2011; accepted 5 December 2011; published online 29 December 2011)

We investigate the energy relaxation of intermolecular motions in liquid water at temperatures ranging from 220 K to 300 K and in ice at 220 K using molecular dynamics simulations. We employ the recently developed frequency resolved transient kinetic energy analysis, which provides detailed information on energy relaxation in condensed phases like two-color pump-probe spectroscopy. It is shown that the energy cascading in liquid water is characterized by four processes. The temperature dependences of the earlier three processes, the rotational-rotational, rotational-translational, and translational-translational energy transfers, are explained in terms of the density of states of the intermolecular motions. The last process is the slow energy transfer arising from the transitions between potential energy basins caused by the excitation of the low frequency translational motion. This process is absent in ice because the hydrogen bond network rearrangement, which accompanies the interbasin transitions in liquid water, cannot take place in the solid phase. We find that the last process in supercooled water is well approximated by a stretched exponential function. The stretching parameter, β, decreases from 1 to 0.72 with decreasing temperature. This result indicates that the dynamics of liquid water becomes heterogeneous at lower temperatures.

© 2011 American Institute of Physics

Article Outline

  1. INTRODUCTION
  2. FREQUENCY RESOLVED TRANSIENT KINETIC ENERGY ANALYSIS
  3. COMPUTATIONAL DETAILS
  4. RESULTS AND DISCUSSION
  5. CONCLUSIONS

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KEYWORDS and PACS

Keywords

electronic density of states, hydrogen bonds, intermolecular mechanics, molecular dynamics method, rotational states, translational states, water

PACS

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.3671993

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

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$abstract.society.value is a Member of CrossRef American Institute of Physics

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