Journal of Chemical Physics, Vol.104, No.6, 2287-2296, 1996
Induced Oscillations in an Electron-Transfer Reaction in the Presence of a Bichromatic Electromagnetic-Field
The effect of a bi-(multi-)chromatic electromagnetic field on electron transfer dynamics in a polar solvent is examined. Whereas the electron population dynamics is characterized by simple exponential decay in the presence of a monochromatic field, a bichromatic field gives rise to large induced coherent oscillations-in electronic density between the reactant and product states; This oscillation is driven indefinitely by the applied field despite the strongly dissipative environment. The dependence of the dynamics on the reaction heat and the laser field properties is explored using an analytical expression derived within the noninteracting blip approximation. The oscillations depend on the held properties : both cosinelike and more complicated behavior can be obtained. For a trichromatic driving force, aperiodic (chaotic) oscillations are found. Ideal conditions and possibly appropriate chemical systems for the experimental verification of this phenomenon are discussed.
Keywords:PHOTOSYNTHETIC REACTION CENTERS;TEMPERATURE-DEPENDENCE;CHARGE RECOMBINATION;EMISSION-SPECTRUM;PROTON-TRANSFER;2-STATE SYSTEM;LASER FIELD;DOUBLE-WELL;DRIVEN;LOCALIZATION