Selective Excitation of Vibrational Wave Packet Motion Using Chirped Pulses

Abstract

Chirped ultrashort pulses are used to selectively excite vibrationally coherent populations in the ground and excited electronic states of a molecule in liquid solution. Negatively chirped pulses are shown to enhance the nonstationary ground state component, while positively chirped pulses discriminate against its formation. Separation of the ground and excited state contributions to the signal allows us to obtain state-specific information about the vibrational dephasing.