Inducing Coherent Oscillations in the Electron Transfer Dynamics of a Strongly Dissipative System with Pulsed Monochromatic Light

Calculations are presented that suggest coherent oscillations in the electronic state populations of an electron transfer reaction in a polar solvent can be induced by subjecting the system to a sequence of monochromatic laser pulses on the picosecond time scale. These oscillations are produced by pumping the system between different steady state distributions attained in the presence and absence of a strong continuous-wave electric field. The amplitude and rise time of these time-dependent oscillations may be altered by changing the pulse duration and the electric field strength. The experimental realization of the proposed scheme will require strong electric fields ({≈}10⁷ V/cm), and the effect will be most pronounced for activationless reactions.