Nonequilibrium relaxation exponentially delays the onset of quantum diffusion

• 成果类型: Article
• 署名作者: Bhattacharyya, Srijan; Sayer, Thomas; Montoya-Castillo, Andres
• 署名单位: University of Colorado System; University of Colorado Boulder; Durham University
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-10121
• DOI: 10.1073/pnas.2424582122
• 发表日期: 2025-05-09
• 关键词: master-equation; transport phenomena; exciton transport; DYNAMICS; mobility; motion

摘要

Predicting the exact many-body quantum dynamics of polarons in materials with strong carrier-phonon interactions presents a fundamental challenge, often necessitating one to adopt approximations that sacrifice the ability to predict the transition from nonequilibrium relaxation to thermodynamic equilibrium. Here, we exploit a recent breakthrough that generalizes the concept of memory beyond its conventional temporal meaning to also encompass space. Specifically, we leverage our finding that the dynamics of observables in systems with local couplings satisfy Green's functions with kernels that are local in time and space. This enables us to employ the dynamics of small lattices over short times to predict the dynamics of thermodynamically large lattices over arbitrarily long timescales while circumventing the deleterious impacts of finite-size effects. We thus interrogate the exact nonequilibrium formation and migration of polarons in one-(1D) and two-dimensional (2D) systems, revealing that their motion approaches diffusive transport only asymptotically in time and system size. We also compare transport in 1D and 2D systems to investigate the effect of dimension in polaron migration physics, illustrating how energy variations can cause localization-a phenomenon observable via current microscopy experiments.