Revealing Hidden Orbital Pathways in Non-Thermal Hot Carrier Relaxation of MXenes via Non-Secular Redfield Quantum Kinetics
Year: 2026
Type: preprint
Abstract: 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 non-thermal 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.
Source: Research Square
Language: English
Subfield: Materials Chemistry
Field: Materials Science
Domain: Physical Sciences
Open Access status: green
Award: G4702742038
OpenAlex ID: W7204199959