Orientation Dynamics of Asymmetric Rotors Using Random Phase Wave Functions

TL;DR

This paper demonstrates that the Random Phase Wave Functions method efficiently models the complex rotational dynamics of asymmetric molecules like SO2 under intense terahertz pulses at ambient temperatures, surpassing traditional computational approaches.

Contribution

It introduces and validates the RPWF method for simulating rotational dynamics of asymmetric top molecules at realistic conditions, where exact methods are computationally infeasible.

Findings

RPWF method becomes more efficient with higher temperature and field strength.

RPWF provides computational access to molecular dynamics beyond exact methods.

The method accurately predicts terahertz-induced rotational responses.

Abstract

Intense terahertz-frequency pulses induce coherent rotational dynamics and orientation of polar molecular ensembles. Exact numerical methods for rotational dynamics are computationally not feasible for the vast majority of molecular rotors - the asymmetric top molecules at ambient temperatures. We exemplify the use of Random Phase Wave Functions (RPWF) by calculating the terahertz-induced rotational dynamics of sulfur dioxide (SO2) at ambient temperatures and high field strengths and show that the RPWF method gains efficiency with the increase in temperature and in the THz-field strengths. The presented method provides wide-ranging computational access to rotational dynamical responses of molecules at experimental conditions which are far beyond the reach of exact numerical methods.