Ultrafast Nonequilibrium Enhancement of Electron-Phonon Interaction in 2 H-MoTe2

Abstract

Understanding nonequilibrium electron-phonon interactions at the microscopic level and on ultrafast timescales is a central goal of modern condensed matter physics. Combining time- and angle-resolved extreme ultraviolet photoemission spectroscopy with constrained density functional perturbation theory, we demonstrate that photoexcited carrier density can serve as a tuning knob to enhance electron-phonon interactions in nonequilibrium conditions. Specifically, nonequilibrium band structure mapping and valley-resolved ultrafast population dynamics in semiconducting transition-metal dichalcogenide 2H-MoTe2 reveal band-gap renormalizations and reduced population lifetimes as photoexcited carrier densities increase. Through theoretical analysis of photoinduced electron and phonon energy and linewidth renormalizations, we attribute these transient features to nonequilibrium modifications of electron-phonon coupling matrix elements. This Letter advances our understanding of microscopic coupling mechanisms enabling control over relaxation pathways in driven solids.