A Windowed Mean Trajectory Approximation for Condensed Phase Dynamics

TL;DR

This paper introduces a novel semiclassical trajectory-based method for simulating condensed phase dynamics, demonstrating high accuracy and robustness across various models and regimes, especially at low temperatures.

Contribution

It presents a new windowed mean trajectory approximation that improves upon existing methods for density matrix propagation in condensed phase systems.

Findings

Outperforms many existing semiclassical methods at low temperatures.

Achieves results comparable to the numerically exact Hierarchical Equations of Motion.

Shows robustness across different models and parameter regimes.

Abstract

We propose a trajectory-based quasiclassical method for approximating dynamics in condensed phase systems. Building upon the previously developed Optimized Mean Trajectory (OMT) approximation that has been used to compute linear and nonlinear spectra, we borrow some ideas from filtering trajectory methods to obtain a novel semiclassical method for the dynamical propagation of density matrices. This new approximation is tested rigorously against standard multistate electronic models, spin-boson model, and models of the Fenna-Matthews-Olson complex. In all instances, the current method is significantly better or as good as many other semiclassical methods available, especially in low-temperature. All results are tested against the numerically exact Hierarchical Equations of Motion method. The new method shows excellent agreement across various parameter regimes with numerically exact results, highlighting the robustness and accuracy of our approach.