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Summary: SPECTROSCOPY IN CRYOCRYSTALS AND MATRICES
Time-resolved CARS measurements of the vibrational decoherence of I2 isolated
in an Ar matrix
M. Karavitis, D. Segale, Z. Bihary, M. Pettersson, and V. A. Apkarian*
Department of Chemistry, University of California Irvine, CA 92697-2025, USA
Fiz. Nizk. Temp. 29, 10711080 SeptemberOctober 2003
Time-resolved coherent anti-Stokes Raman scattering is applied to prepare and interrogate
vibrational coherences on the ground electronic surface of molecular iodine isolated in Ar matrices.
The coherence decay time shows a linear dependence on vibrational quantum numbers for
v 315. The temperature dependence of decoherence rates is negligible for v 7 in
the experimental range T 1832 K. For a v 13, 14 superposition, the temperature dependence
indicates dephasing by a 66 cm 1
pseudo-local phonon, just outside the Debye edge of the
solid. The accuracy of the data is limited due to two-photon induced dissociation of the molecule,
a process which is characterized using polarized fields. The T0 limit of dephasing is
discussed. © 2003 American Institute of Physics. DOI: 10.1063/1.1614200
1. INTRODUCTION
In a recent paper we reported time-resolved coherent
anti-Stokes Raman scattering TRCARS measurements on
I2 isolated in an Ar matrix.1
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