Trajectory-based non-adiabatic simulations of the polariton relaxation dynamics DOI
Deping Hu,

Benjamin X. K. Chng,

Wenxiang Ying

et al.

The Journal of Chemical Physics, Journal Year: 2025, Volume and Issue: 162(12)

Published: March 27, 2025

We benchmark the accuracy of various trajectory-based non-adiabatic methods in simulating polariton relaxation dynamics under collective coupling regime. The Holstein–Tavis–Cummings Hamiltonian is used to describe hybrid light–matter system N molecules coupled a single cavity mode. apply recently developed simulate population by initially exciting upper state and results against populations computed from exact quantum dynamical propagation using hierarchical equations motion approach. In these benchmarks, we have systematically varied number N, detunings, strengths. Our demonstrate that symmetrical quasi-classical method with γ correction spin-mapping linearized semi-classical approaches yield more accurate than traditional mixed quantum-classical methods, such as Ehrenfest surface hopping techniques.

Language: Английский

Polariton spectra under the collective coupling regime. II. 2D non-linear spectra DOI
M. Mondal, A. Nick Vamivakas, Steven T. Cundiff

et al.

The Journal of Chemical Physics, Journal Year: 2025, Volume and Issue: 162(7)

Published: Feb. 20, 2025

In our previous work [Mondal et al., J. Chem. Phys. 162, 014114 (2025)], we developed several efficient computational approaches to simulate exciton–polariton dynamics described by the Holstein–Tavis–Cummings (HTC) Hamiltonian under collective coupling regime. Here, incorporated these strategies into previously Lindblad-partially linearized density matrix (L-PLDM) approach for simulating 2D electronic spectroscopy (2DES) of particular, apply quantum propagation scheme in Paper I both forward and backward propagations PLDM develop an importance sampling graphics processing unit vectorization that allow us reduce costs from O(K2)O(T3) O(K)O(T0) 2DES simulation, where K is number states T time steps propagation. We further simulated HTC regime analyzed signal rephasing non-rephasing contributions ground state bleaching, excited emission, stimulated emission pathways.

Language: Английский

Citations

1
Trajectory-based non-adiabatic simulations of the polariton relaxation dynamics DOI
Deping Hu,

Benjamin X. K. Chng,

Wenxiang Ying

et al.

The Journal of Chemical Physics, Journal Year: 2025, Volume and Issue: 162(12)

Published: March 27, 2025

We benchmark the accuracy of various trajectory-based non-adiabatic methods in simulating polariton relaxation dynamics under collective coupling regime. The Holstein–Tavis–Cummings Hamiltonian is used to describe hybrid light–matter system N molecules coupled a single cavity mode. apply recently developed simulate population by initially exciting upper state and results against populations computed from exact quantum dynamical propagation using hierarchical equations motion approach. In these benchmarks, we have systematically varied number N, detunings, strengths. Our demonstrate that symmetrical quasi-classical method with γ correction spin-mapping linearized semi-classical approaches yield more accurate than traditional mixed quantum-classical methods, such as Ehrenfest surface hopping techniques.

Language: Английский

Citations

0