Picosecond holographic-grating spectroscopy.
Interfering light waves produce an optical interference pattern in any medium that interacts with light. This modulation of some physical parameter of the system acts as a classical holographic grating for optical radiation. When such a grating is produced through interaction of pulsed light waves with an optical transition, a transient grating is formed whose decay is a measure of the relaxation time of the excited state. Transient gratings can be formed in real space or in frequency space depending on the time ordering of the interfering light waves. The two gratings are related by a space-time transformation and contain complementary information on the optical dynamics of a system. The status of a grating can be probed by a delayed third pulse, which diffracts off this grating in a direction determined by the wave vector difference of the interfering light beams. This generalized concept of a transient grating can be used to interpret many picosecond-pulse optical experiments on condensed-phase systems. Examples of some low-temperature experiments will be presented. In principle, many of these experiments could also be performed by using stochastic broad-band excitation. In these nonlinear photon-interference experiments the time resolution is determined by the correlation time of the light source rather than its pulse width.
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