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PROOF COPY 015417JCP Onset of decoherence: Six-wave mixing measurements of vibrational
 

Summary: PROOF COPY 015417JCP
PROOF
COPY
015417JCP
Onset of decoherence: Six-wave mixing measurements of vibrational
decoherence on the excited electronic state of I2 in solid argon
Z. Bihary, M. Karavitis, and V. Ara Apkariana)
Department of Chemistry, University of California, Irvine, California 92697
Received 20 October 2003; accepted 10 February 2004
Pump­probe, four-wave, and six-wave mixing measurements of I2 isolated in solid argon are used
to provide a clear experimental measure for the onset of vibrational quantum decoherence on the
excited electronic state. The electronically resonant, six-wave mixing measurements bypass the
rapid electronic dephasing, and measure the quantum cross-correlation between two packets
launched on the B-state. The vibrational quantum coherence survives 1 period of motion, 400 fs,
during which 2000 cm 1
of energy is transferred to the lattice. The decoherence occurs during the
second cycle of motion, while classically coherent motion measured via pump­probe spectroscopy
using the same electronic resonances continues for 15 periods. This is contrasted with vibrational
dephasing on the ground electronic surface, which lasts for 102
periods, as measured through

  

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

 

Collections: Chemistry