Web Release Date: April 17,
Using the Phase of Light as a Photochemical Tool
Department of Chemistry (m/c 111), University of Illinois at Chicago, 845 West Taylor Street, Chicago, Illinois 60607-7061
Steacie Institute for Molecular Sciences, National Research Council of Canada, Ottawa K1A 0R6, Canada
Received: October 23, 2000
In Final Form: January 17, 2001
Abstract:
It is shown both theoretically and experimentally that the phase of a transition dipole matrix element may be determined from the interference between competing quantum mechanical paths. Specifically, we consider simultaneous m- and n-photon excitation of a molecule to a degenerate continuum state, leading to multiple reaction products. Variation of the relative phase of the electromagnetic fields produces a modulation of the product signals in the various channels. A relation between the phase lag between a pair of product signals and properties of the continuum is established. Information is revealed about coupling mechanisms, the properties of weak spectroscopic transitions, and the phases of quasi-bound wave functions.
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