Pulsed laser preparation and quantum superposition state evolution in regular and irregular systems

Abstract

The nature of the prepared state is crucial to an understanding of isolated-molecule intramolecular dynamics. A model is utilized to compare the created quantum superposition state in pulsed laser excitation from (1) a ground electronic state with regular nuclear wavefunctions to an excited electronic state with regular nuclear wavefunctions with that from (2) the regular ground state to an excited state with irregular nuclear wavefunctions. All results are in the quantum-mechanical small-molecule limit. Visual inspection of the created state and its evolution shows distinct qualitative differences in these two cases, although various theoretically studied quantities do not reveal an obvious distinction. The differences are expected to be experimentally observable in tirne-resolved emission.

Excitation, dynamics, and control of rotationally autoionizing Rydberg states of H2

“…͑6͒ we obtain the corresponding rotating and counterrotating wave components of the complex excitation function, i.e., cef͑ ns , t͒ = cef + ͑ ns , t͒ + cef − ͑ ns , t͒. By straightforward extension of the analytical results by Brumer, Shapiro and Taylor 16,17,27 we find a solution for a Gaussian pulse centered at an arbitrary time t k , which will allow for analytic treatment of sequences of pulses. The cef is given by the equations…”

Saddle scars: existence and applications

“…When this happens one says that the quantum state is scarred by the unstable periodic orbit or that one has a quantum scar. Such states have been observed at first in numerical simulations [4] [5] [6] and, more recently, experimental evidence was found [7] on a semiconductor quantum-well tunneling experiment.…”

A generalized approach to the control of the evolution of a molecular system

“…We assume that the molecule-field coupling is dominated by the dipole transition interaction V nk ϭϪ nk E, where nk is the transition dipole matrix element. Of course, nk ϭ el f nk , where f nk ϭ ͐dru n *(r)u k (r) is the Franck-Condon factor between electronic surfaces n and k. 28 The resonant continuous electric field E(t) can be written in the form…”