Abstract
A novel coherent spectroscopy is applied to measure ultrafast vibrational relaxation. Its performance is quantitatively evaluated through computer simulations. Transient Resonant Impulsive Stimulated Raman Scattering (TRISRS), is used to record vibrational relaxation in rapidly evolving nascent , following photodissociation of in solution. The TRISRS experiment involves a sequence of three pulses. A primary UV photolyzing pulse at 308 nm initiates triiodide dissociation. At a certain delay with respect to the photolysis a secondary intense 'push' pulse at 616 nm sets in motion ground state coherent vibration. Its decay is followed via periodic transmission modulations of a continuously delayed tunable probing pulse1. In essence these modulations record a Raman Free Induction Decay (FID) whose duration defines the minimum time that a dynamic variable must be followed in order to reconstruct its power spectrum. Master simulations of vibrational relaxation, coupled to quantum wave-packet representation of the light-matter interaction2, are combined to provide a quantitative analysis of the experimental results.
© 1994 Optical Society of America
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