Energy relaxation versus spectral diffusion of the OH-stretching vibration of HOD in liquid-to-supercritical deuterated water

J Chem Phys. 2005 Oct 22;123(16):161105. doi: 10.1063/1.2110087.

Abstract

The dynamics of vibrational energy relaxation (VER) of the OH-stretching vibration of HOD in liquid-to-supercritical heavy water is studied as a function of temperature and solvent density by femtosecond mid-infrared spectroscopy. Using the dielectric constant of the fluid both, the OH-stretching absorption frequency and the VER rate, can be correlated phenomenologically with the average hydrogen-bond connectivity within the random D2O network. This correlation enables the identification of thermodynamic conditions under which spectral diffusion due to hydrogen-bond breakage/formation is much faster than VER.

MeSH terms

  • Chemistry, Physical / methods*
  • Deuterium / chemistry*
  • Diffusion
  • Hydrogen Bonding
  • Hydroxides / chemistry*
  • Solvents / chemistry
  • Spectrophotometry, Infrared / methods
  • Spectrum Analysis / methods
  • Temperature
  • Thermodynamics
  • Water / chemistry*

Substances

  • Hydroxides
  • Solvents
  • Water
  • hydroxide ion
  • Deuterium