Single-shot measurement of ultrafast time-varying phase modulation induced by femtosecond laser pulses with arbitrary polarization

We demonstrate a single-shot measurement of the transient phase modulation due to field free molecular alignment at the revival times of a rotational wave packet. The wave packet is excited by an arbitrarily polarized ultrashort laser pulse in CO2 at room temperature. With this technique the time dependence along the eigenpolarization directions of the linear susceptibility tensor, i.e., the time dependence of its principle components, can be directly observed with high sensitivity.