Electron Correlation via Frozen Gaussian Dynamics

TL;DR

This paper assesses the semiclassical Frozen Gaussian method's effectiveness in simulating correlated electron dynamics, highlighting its potential and current limitations for real-time electron behavior modeling.

Contribution

It introduces a combined exact-exchange and semiclassical correlation approach for electron dynamics and evaluates its performance on model systems.

Findings

The method accurately captures certain correlated electron behaviors.

Challenges remain in broad applicability due to identified limitations.

Potential for improved electron dynamics simulations with further development.

Abstract

We investigate the accuracy and efficiency of the semiclassical Frozen Gaussian method in describing electron dynamics in real time. Model systems of two soft-Coulomb-interacting electrons are used to study correlated dynamics under non-perturbative electric fields, as well as the excitation spectrum. The results show that a recently proposed method that combines exact-exchange with semiclassical correlation to propagate the one-body density-matrix holds promise for electron dynamics in many situations that either wavefunction or density-functional methods have difficulty describing. The results also however point out challenges in such a method that need to be addressed before it can become widely applicable.