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Abstract
Theoretical treatments of laser-induced inelastic scattering have traditionally considered (translational) free-to-free transitions. We present a treatment of laser-induced resonances (quasibound states) in molecular scattering. The main result is that large cross sections for inelastic scattering may be achieved at low radiation densities, fully exploiting the monochromaticity and tunability of lasers. A calculation is performed which models the collision of Xe and F atoms in the presence of two lasers. One laser dresses the molecular electronic states, inducing the formation of scattering resonances; the other serves as a probe, inducing transitions between resonances during the collision (energy transfer). The system finally breaks apart by stimulated emission and with an increase in translational energy (laser heating). The total scattering cross section is high (∼ 1 Å2), even though both lasers are of low intensity (less than 1 kW cm-2). Applications to spectroscopy of the transition state and to curve-switching processes are discussed.
This work was supported in part by the Air Force Office of Scientific Research (AFSC), United States Air Force, under Grant AFOSR 82-0046 and the National Science Foundation under Grant No. CHE-8022874. The United States Government is authorized to reproduce and distribute reprints for governmental purposes notwithstanding any copyright notation hereon. One of us (TFG) acknowledges the Camille and Henry Dreyfus Foundation for a Teacher-Scholar Award (1975–82).
This work was supported in part by the Air Force Office of Scientific Research (AFSC), United States Air Force, under Grant AFOSR 82-0046 and the National Science Foundation under Grant No. CHE-8022874. The United States Government is authorized to reproduce and distribute reprints for governmental purposes notwithstanding any copyright notation hereon. One of us (TFG) acknowledges the Camille and Henry Dreyfus Foundation for a Teacher-Scholar Award (1975–82).
Notes
This work was supported in part by the Air Force Office of Scientific Research (AFSC), United States Air Force, under Grant AFOSR 82-0046 and the National Science Foundation under Grant No. CHE-8022874. The United States Government is authorized to reproduce and distribute reprints for governmental purposes notwithstanding any copyright notation hereon. One of us (TFG) acknowledges the Camille and Henry Dreyfus Foundation for a Teacher-Scholar Award (1975–82).