Rotational dynamics of an asymmetric top molecule in parallel electric and non-resonant laser fields

TL;DR

This paper theoretically investigates the rotational behavior of asymmetric top molecules under combined electric and laser fields, highlighting non-adiabatic effects and conditions for adiabatic control, using benzonitrile as a model.

Contribution

It provides a detailed analysis of non-adiabatic effects in the rotational dynamics of asymmetric top molecules in combined fields and identifies parameters for adiabatic control.

Findings

Formation of pendular doublets causes non-adiabatic effects

Avoided crossings between energy levels influence dynamics

Specific field parameters enable adiabatic rotational control

Abstract

We present a theoretical study of the rotational dynamics of asymmetry top molecules in an electric field and a parallel non-resonant linearly polarized laser pulse. The time-dependent Schr\"odinger equation is solved within the rigid rotor approximation. Using the benzonitrile molecule as prototype, we investigate the field-dressed dynamics for experimentally accessible field configurations and compare these results to the adiabatic predictions. We show that for an asymmetric top molecule in parallel fields, the formation of the pendular doublets and the avoided crossings between neighboring levels are the two main sources of non-adiabatic effects. We also provide the field parameters under which the adiabatic dynamics would be achieved.