Coherent interference of molecular electronic states in NO by two-color femtosecond laser pulses

Abstract

Quantum coherence interference between electronic states in molecules is an important factor for controlling electronic and nuclear dynamics in photoinduced physics and chemistry. We measure and model molecular angle-dependent photoionization yields to explore coherent interference dynamics between quasiequal energy electronic-vibrational states of the nitric oxide molecule, NO, by ultrafast phase-controlled two-color femtosecond laser pulses. We demonstrate by experiment and theory that the photoelectron angular distribution of NO, where two excited electronic states are coherently combined by ultrafast pulses, is a function of the relative phase of the pulses, and the photoelectron kinetic energy. The modification of photoelectron emission angular patterns encodes the information of the coherence via electronic state interference. The result allows access to phase-dependent state correlations and ultrafast vibrationic dynamics in molecules.