A windowed mean trajectory approximation for condensed phase dynamics

We propose a trajectory-based quasi-classical method for approximating dynamics in condensed phase systems. Building upon the previously developed optimized mean trajectory 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 models, and models of the Fenna-Matthews-Olson complex. For dissipative systems, the current method is significantly better or as good as many other semiclassical methods available, especially at low temperatures and for off-diagonal density matrix elements, whereas for scattering models, the current method bears similar limitations as mean-field propagation schemes. 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.

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Publication Details

Journal
The Journal of Chemical Physics
Published
2024-12-04
DOI
https://doi.org/10.1063/5.0234653
Primary Topic
Spectroscopy and Quantum Chemical Studies
Type
article
Field-Weighted Citation Impact
0.00

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article

A windowed mean trajectory approximation for condensed phase dynamics

Kritanjan Polley
The Journal of Chemical Physics
Spectroscopy and Quantum Chemical Studies
article

A windowed mean trajectory approximation for condensed phase dynamics

Kritanjan Polley
article en

Abstract

We propose a trajectory-based quasi-classical method for approximating dynamics in condensed phase systems. Building upon the previously developed optimized mean trajectory 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 models, and models of the Fenna-Matthews-Olson complex. For dissipative systems, the current method is significantly better or as good as many other semiclassical methods available, especially at low temperatures and for off-diagonal density matrix elements, whereas for scattering models, the current method bears similar limitations as mean-field propagation schemes. 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.

The Journal of Chemical PhysicsVol. 161(21)
Lawrence Berkeley National Laboratory (US), University of California, Berkeley (US)
U.S. Department of Energy
Openalex Percentile: Top 80%
Spectroscopy and Quantum Chemical Studies
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A windowed mean trajectory approximation for condensed phase dynamics — Kritanjan Polley · The Journal of Chemical Physics (2024) | TGRS Research Map | TGRS