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Spectral inhomogeneity induced by vacancies and thermal phonons and associated observables in time-and frequency-domain nonlinear
 

Summary: Spectral inhomogeneity induced by vacancies and thermal phonons
and associated observables in time- and frequency-domain nonlinear
spectroscopy: I2 isolated in matrix argon
Z. Bihary and M. Karavitis
Department of Chemistry, University of California, Irvine, California 92697-2025
R. B. Gerber
Department of Chemistry, University of California, Irvine, California 92697-2025
and Department of Physical Chemistry, The Hebrew University, Jerusalem, 91904, Israel
V. A. Apkariana)
Department of Chemistry, University of California, Irvine, California 92697-2025
Received 9 July 2001; accepted 15 August 2001
The vibrational self-consistent field method is used to analyze the inhomogeneous spectral
distribution of transitions caused by vacancies and thermally populated phonons, specializing to
molecular iodine isolated in an Ar matrix. At experimentally relevant temperatures, for a vacancy
concentration of 1.4%, both defect-induced and phonon-induced spectral shifts contribute to the
spectral distribution. Both contributions scale linearly with vibrational overtone number. The
predicted widths are consistent with reported resonant Raman spectra. In time-resolved coherent
anti-Stokes Raman scattering TRCARS measurements, spectral indistinguishability implies that
all members of the inhomogeneous ensemble contribute coherently to the detectable homodyne
signal. The connection between spectral distribution and the observable in TRCARS is derived. The

  

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

 

Collections: Chemistry