Trajectory Ensemble Methods Provide Single-Molecule Statistics for Quantum Dynamical Systems

• DOI: 10.1021/acs.jctc.1c00477
• Publication Date: 2022-03-01T17:09:30Z
• Authors: Amro Dodin; Justin Provazza; David F. Coker; Adam P. Willard
• Keywords: Statistical ensemble; Ensemble average; Quantum system; Microcanonical ensemble

The emergence of experiments capable probing quantum dynamics at the single-molecule level requires development new theoretical tools simulating and analyzing these beyond an ensemble-averaged description. In this article, we present efficient method for sampling individual systems that make up ensemble apply it to study nonequilibrium ubiquitous spin-boson model. We generate single-system trajectories, analyze trajectory using from classical statistical mechanics. Our results demonstrate coherence is highly heterogeneous due variations in initial bath configuration, which significantly affects transient exchange between system its bath. observe single tend retain over time scales longer than ensemble. also compute a novel thermodynamic entanglement entropy quantifies driving force favoring system-bath entanglement.