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J. Phys. Chem. 1995, 99, 1453-7465 7453 Femtosecond Many-Body Dynamics of Caging: Experiment and Simulation of 12
 

Summary: J. Phys. Chem. 1995, 99, 1453-7465 7453
Femtosecond Many-Body Dynamics of Caging: Experiment and Simulation of 12
Photodissociation-Recombination in Solid Ar
Z. Li, R. Zadoyan, V. A. Apkarian," and C. C. Martens*
Department of Chemistry, University of Califomia, Imine, Califomia 92717-2025
Received: October 20, 1994; In Final Form: February IO, I995@
The many-body dynamics resulting from I2 photodissociation in solid Ar are investigated using a combination
of time-resolved pump-probe measurements and molecular dynamics simulations. The wavelength dependence
of the signals, measured with a time resolution of 120-150 fs, are reported. Polarization experiments indicate
that, for the duration of observation, the photodissociation-recombination proceeds adiabatically. Molecular
dynamics simulations, combined with the classical Franck principle, are employed to calculate simulated
signals, which agree well with experiment. The microscopic dynamics of the system are then investigated
by examining individual trajectory data in detail, giving an atomic-scale view of the photoinduced dissociation
of IZon the A excited electronic surface, the subsequent caging of the photofragments by the lattice, I2
recombination, and coherent vibrational dynamics of the nascent diatomic molecule. Recombination is found
to be a dynamically complex process, involving bidirectional energy flow between molecule and lattice during
the early time motion of the photofragments in the solvent cage. The recombination event, when defined as
the permanent deexcitation of the IZbelow its dissociation threshold, is not directly associated with any
prominent feature in the pump-probe signal.
I. Introduction

  

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

 

Collections: Chemistry