Spectroscopic and quantum‐control aspects of ultrashort‐pulse synthesis through impulsive high‐order stimulated Raman scattering

Abstract

AbstractThe spectroscopic and quantum‐control aspects of short‐pulse synthesis through the generation of multiple Stokes and anti‐Stokes sidebands in an impulsively pre‐excited Raman‐active medium are considered. The use of sequences of short laser pulses leading to a resonant excitation of Raman modes is shown to allow the generation of multiple Stokes and anti‐Stokes sidebands to be considerably enhanced, with the characteristic length of the spectral broadening of a probe pulse propagating in a Raman‐active medium pre‐excited by a sequence of short pulses being inversely proportional to the number of pulses in this sequence. Coherent four‐wave mixing techniques are shown to be a convenient tool for visualizing the result of impulsive preparation of a Raman‐active medium. The results of Raman spectroscopic studies are used to specify Raman‐active molecules with sufficiently short periods of Raman vibrations and high efficiencies of Raman scattering, which offer especially much promise for the generation of few‐cycle light pulses in Raman‐active media. Copyright © 2002 John Wiley & Sons, Ltd.