Eliminating molecular-alignment dephasing with a phase-modulated femtosecond laser pulse

Abstract

Alignment dephasing caused by centrifugal distortion is a significant effect accompanying laser-induced field-free molecular alignment. Centrifugal distortion is the manifestation of the intrinsic nonrigidity of molecules, which is especially prominent when molecules are excited to high angular velocities. In this work, we show that this type of dephasing can be almost completely eliminated by modulating the phase of the femtosecond laser pulse. Nearly perfect molecular alignment can be achieved as if the molecules were ideal rigid rotors. The dephasing effect can be cancelled in various time windows by tuning the modulation strength parameter. The dephasing cancellation mechanism is explained by considering the relative phases of the eigenstates forming the rotational wave packet. This work is of great significance to the experiment and dynamics studies of molecular alignment.