EXTRACTING SIGNATURES OF QUANTUM CHAOS FROM THE TIME-RESOLVED FLUORESCENCE OF ISOLATED MOLECULES

We show how to extract a statistically significant temporal signature of quantum chaos from the fluorescence decay of mixed molecular states prepared by multimode partially coherent laser pulses, Specifically, the average fluorescence from appropriately prepared molecules is show n to be an incoherently averaged quantity which, aside from radiative damping factors, is linearly related to the transient part of the aver age survival probability which distinguishes regular from irregular vi brational dynamics. A three step procedure is developed for removing t he masking effect of radiative damping, thereby allowing a direct extr action of a dynamical signature of quantum chaos, Simulated fluorescen ce signals with regular and irregular vibrational dynamics are analyze d to demonstrate the effectiveness of this approach and to motivate ex perimental studies. (C) 1997 American Institute of Physics.