Non-adiabatic effects in long-pulse mixed-field orientation of a linear polar molecule

TL;DR

This paper theoretically investigates how combined electrostatic and laser fields influence the rotational behavior of linear molecules, highlighting the importance of non-adiabatic effects in mixed-field orientation experiments.

Contribution

It provides a detailed analysis of non-adiabatic effects in mixed-field molecular orientation, offering insights into field parameters needed for adiabatic control.

Findings

Non-adiabatic effects are significant in typical experimental conditions.

Time-dependent modeling is essential for accurate description of molecular dynamics.

Field parameters can be tuned to achieve adiabatic behavior.

Abstract

We present a theoretical study of the impact of an electrostatic field combined with non-resonant linearly polarized laser pulses on the rotational dynamics of linear molecules. Within the rigid rotor approximation, we solve the time-dependent Schr\"odinger equation for several field configurations. Using the OCS molecule as prototype, the field-dressed dynamics is analyzed in detail for experimentally accessible static field strengths and laser pulses. Results for directional cosines are presented and compared to the predictions of the adiabatic theory. We demonstrate that for prototypical field configuration used in current mixed-field orientation experiments, the molecular field dynamics is, in general, non-adiabatic, being mandatory a time-dependent description of these systems. We investigate several field regimes identifying the sources of non-adiabatic effects, and provide the field parameters under which the adiabatic dynamics would be achieved.