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Time resolved coherent anti-Stokes Raman scattering of I2 isolated in matrix argon: Vibrational dynamics on the ground electronic state
 

Summary: Time resolved coherent anti-Stokes Raman scattering of I2 isolated
in matrix argon: Vibrational dynamics on the ground electronic state
M. Karavitis, R. Zadoyan, and V. Ara Apkariana)
Department of Chemistry, University of California, Irvine, California 92697-2025
Received 16 August 2000; accepted 14 December 2000
Time-resolved, electronically resonant, coherent anti-Stokes Raman scattering is used to prepare
and interrogate vibronic coherences of molecular iodine in matrix Ar. Coherences that involve
evolution on the excited B(3
0u) state, first- and third-order coherences, decay in less than one
vibrational period 300 fs . In contrast, as many as 200 vibrational periods of motion can be
observed for Raman-prepared wave packets consisting of zero-phonon vibrational superpositions on
the ground electronic state second-order coherence . Packets consisting of v 4, 5 and v 3, 4, 5
on the X(1
g) state decay with a half-life of 10 1 ps at 31 K, allowing a more accurate measure
of vibrational level spacings and decoherence time than has been possible in frequency domain. The
harmonic frequency of the molecule is reduced by 1.5 cm 1
0.7% in the matrix. The lack of
recurrence in the excited electronic state ensures that the resonant anti-Stokes scattering arises only
from the negative momentum component of the Raman packet. This momentum filter, which should
be ubiquitous in condensed media, leads to a signal with deeper modulation than in the gas phase.

  

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

 

Collections: Chemistry