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Vibrational dissipation and dephasing of I2(v = 119) in solid Kr Michael Karavitis, Takayuki Kumada, Ilya U. Goldschleger and V. Ara Apkarian*
 

Summary: Vibrational dissipation and dephasing of I2(v = 119) in solid Kr
Michael Karavitis, Takayuki Kumada, Ilya U. Goldschleger and V. Ara Apkarian*
Department of Chemistry, University of California, Irvine, CA, 92697-2025, USA
Received 19th October 2004, Accepted 18th January 2005
First published as an Advance Article on the web 1st February 2005
Time- and frequency-resolved coherent anti-Stokes Raman scattering is used to carry out systematic measure-
ments of vibrational dephasing on I2(v 119) isolated in solid Kr, as a function of temperature, T 745 K.
The observed quantum beats, ov0
,v00 allow an accurate reconstruction of the solvated molecular potential, which is
well represented by the Morse form: oe 211.56 0.14, oexe 0.658 0.006. Near T 7 K, the coherence
decay rates gv,0 become independent of temperature and show a linear v-dependence, indicative of dissipation,
which must be accompanied by the simultaneous creation of at least four phonons. At higher temperatures, the
T-dependence is exponential and the v-dependence is quadratic, characteristic of pure dephasing via pseudo-local
phonons. A normal mode analysis suggests librations as the principle modes responsible for pure dephasing.
1. Introduction
Vibrational phase and energy transfer in condensed media, in
the liquid phase1,2
and in the solid state,3
are fundamental
building blocks of many-body dynamics. The more modern

  

Source: Apkarian, V. Ara - Department of Chemistry, University of California, Irvine

 

Collections: Chemistry