通过非久期Redfield量子动力学揭示MXenes非热热载流子弛豫中的隐藏轨道路径

中文摘要 AI 辅助

非热载流子弛豫通常从布居动力学或光谱可观测量中推断出来，但这两类量均无法唯一确定能量与相干性重新分布的微观通道。我们引入了一种路径分辨的量子动力学框架，该框架可同时将超快弛豫投影到轨道布居、轨道间能流、相干性、光谱可见度以及动力学转移网络的隐藏路径扇区上。将该框架应用于MXenes，揭示出强烈非均匀的轨道再分布，以及材料特有的微观转移通道层级结构。温度、激发振幅和耗散参数会调控路径竞争与光谱振幅，同时使主导通道的特性基本保持不变。瞬时能流、累积转移、相干性和光谱可见度呈现出不等价的层级排序，这种不等价性分离出一组隐藏路径，尽管其常规光谱信号微弱，但在动力学上仍具有重要意义。由此得到的时-能相干性表征将非热弛豫重构为包含可观测和隐藏扇区的结构化动力学网络，从而为解析受驱动量子材料中的微观能量转移路径提供了通用方法。

英文摘要

Non-thermal carrier relaxation is routinely inferred from population dynamics or spectroscopic observables, yet neither class of quantity uniquely identifies the microscopic channels through which energy and coherence are redistributed. We introduce a pathway-resolved quantum-kinetic framework that simultaneously projects ultrafast relaxation onto orbital populations, directional inter-orbital transferes, coherence, spectroscopic visibility, and a hidden-pathway sector of the dynamical transfer network. Application to MXenes exposes strongly non-uniform orbital redistribution together with material-specific hierarchies of microscopic transfer channels. Temperature, excitation amplitude, and dissipative parameters modulate pathway competition and spectral amplitudes while leaving the identity of the dominant channels largely intact. Instantaneous transfer contributions, cumulative directional transfer, coherence, and spectroscopic visibility are shown to follow inequivalent hierarchical orderings. This non-equivalence isolates a set of hidden pathways that remain dynamically consequential despite weak conventional spectroscopic signatures. The resulting time energy coherence representation recasts nonthermal relaxation as a structured dynamical network comprising observable and hidden sectors, thereby providing a general methodology for resolving microscopic orbital transfer pathways in driven quantum materials.

发表机构

• University of Tehran（德黑兰大学）
• Southern University of Science and Technology（南方科技大学）

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