Abstract

The rapidly advancing area of computer simulation for quantum-mechanical systems now permits the direct evaluation of spectroscopic observables for condensed phase systems, which increasingly overlaps frontier ultra-fast measurements. In this paper recent theoretical techniques are outlined and representative results from application to the hydrated electron are described that exemplify the close connection between theory and experiment that can now be made. Results focus, first, on the decomposition of the equilibrium optical spectrum into the underlying electronic excitations and on simulation of a proposed photophysical hole-burning experiment designed to test the veracity of this decomposition. Second, the author examines aspects of the transient relaxation of initially nonequilibrium photogenerated electrons by simulation of the spectroscopic signature of proposed early time states and of the relaxation of these states to equilibrium.

© 1990 Optical Society of America

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