OPTICAL IMPULSIVE EXCITATION OF MOLECULAR PSEUDOROTATION IN JAHN-TELLER SYSTEMS

We analyze the use of vibrationally abrupt nonresonant laser pulses to prepare coherently pseudorotating states in a model Jahn-Teller molecule. Our derivation of impulsive excitation invokes the dynamical adiabatic phase for the perturbed electronic ground state. Polarization selection between two Raman active distortion coordinates allows creation of an orbit of arbitrary eccentricity. Repetition of the pulse pair at the pseudorotational frequency amplifies the nuclear motion. Timing of a resonant pulse of given polarization, or choice of polarization for a given delay, transfers the moving wave packet to either or both Jahn-Teller branches of an electronic excited state. © 1990 American Institute of Physics.