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Interrogation and control of condensed phase chemical dynamics with linearly chirped pulses: I2 in solid Kr
 

Summary: Interrogation and control of condensed phase chemical dynamics
with linearly chirped pulses: I2 in solid Kr
M. Sterling, R. Zadoyan, and V. A. Apkarian
Department of Chemistry, University of California, Irvine, California 92717
Received 19 October 1995; accepted 30 January 1996
The effect of linearly chirped pulses in condensed phase ultrafast pump­probe experiments is
investigated by classical simulations for the model system of I2 isolated in a Kr matrix. The central
frequency of the probe laser is selected to monitor exclusively the event of first collision and recoil
of atoms from the host cage. It is shown that a chirped probe pulse enables characterization of the
magnitude and sign of the momentum of the evolving trajectory flux. This can be understood by
transforming the frequency­time profile of the probe pulse to coordinate­time space, and noting
that the observable signal is a function of the relative group velocities of the traveling wave packet
and the traveling window function. The effect of the pump pulse chirp, is a measure of the
controllability of the evolving dynamics. In the particular case studied, breaking and remaking of the
I2 bond near the dissociation limit of the bare molecule, it is shown that the memory of the system
outlasts the collision with the cage. Negatively chirped pulses produce a more tightly focused wave
packet during recoil, leading to a stronger population coherence in the subsequent dynamics.
© 1996 American Institute of Physics. S0021-9606 96 02317-2
INTRODUCTION
The availability of lasers with ultrashort pulses naturally

  

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

 

Collections: Chemistry