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Summary: Faraday Discuss., 1997, 108, 255È269
Lattice dynamics from the "eyesÏ of the chromophore
Real-time studies of isolated in rare gas matricesI
2
R. Zadoyan, J. Almy and V. A. Apkarian*
Department of Chemistry, University of California, Irvine, CA 92697-2025, USA
Molecular iodine isolated in rare gas solids is used as a model system to
develop the framework for interpretation of condensed phase pumpÈprobe
observables, specializing in information content regarding multi-body
dynamics. The principles are illustrated through a series of examples, where,
beside the molecular vibronic coherence, the cage motions can be directly
dissected. The large variety of behaviors which can be staged in this system
include: elastic cage recoil, highly non-linear and dissipative cage response,
long-lived cage coherence driven through guestÈhost resonances, nearly
decoupled guestÈhost dynamics, and cage induced dynamical solvation of
electronic surfaces. Although the underlying dynamics can be understood in
great depth when aided by simulations, we attempt a clear distinction
between direct experimental observables and inferences based on simula-
tions.
1 Introduction
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