Multiconfigurational Mixed Quantum-Classical Approach for Correlated Many-Body Dynamics

Abstract

In this work, we introduce a multiconfigurational mixed quantum-classical many-body approach for simulating the finite-temperature correlated multi-exciton dynamics in the presence of phonon-induced static and dynamic disorder. In this mixed quantum-classical approach, the excitonic subsystem is described using a multiconfigurational wavefunction that extends beyond the mean-field limit, while the phonons are evolved quasi-classically. Using this approach, we simulate a multi-excitonic dissipative system and show how the interplay between phonon-induced dynamic disorder and exciton-exciton many-body interactions determines excitation-dependent excitonic transport and spatial correlations. Our results show that while the mean-field approach produces semi-quantitatively accurate diffusive dynamics, it does not capture the spatial correlations as expected. We find that a mean-field path approximation, where we generate pre-computed trajectories using our mean-field mixed quantum-classical approach and then perform multiconfigurational dynamics, can reproduce the spatial correlations to a good accuracy, positioning this approach as an efficient method for capturing spatial correlations in complex systems.