Simultaneous Observation of Carrier-Specific Redistribution and Coherent Lattice Dynamics in 2H-MoTe<sub>2</sub> with Femtosecond Core-Level Spectroscopy.

Attar, Andrew R; Chang, Hung-Tzu; Britz, Alexander; Zhang, Xiang; Lin, Ming-Fu; Krishnamoorthy, Aravind; Linker, Thomas; Fritz, David et al. · ACS Nano · 2020

basic_science · Level V

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Abstract

We employ few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy to reveal simultaneously the intra- and interband carrier relaxation and the light-induced structural dynamics in nanoscale thin films of layered 2H-MoTe<sub>2</sub> semiconductor. By interrogating the valence electronic structure via localized Te 4<i>d</i> (39-46 eV) and Mo 4<i>p</i> (35-38 eV) core levels, the relaxation of the photoexcited hole distribution is directly observed in real time. We obtain hole thermalization and cooling times of 15 ± 5 fs and 380 ± 90 fs, respectively, and an electron-hole recombination time of 1.5 ± 0.1 ps. Furthermore, excitations of coherent out-of-plane A<sub>1g</sub> (5.1 THz) and in-plane E<sub>1g</sub> (3.7 THz) lattice vibrations are visualized through oscillations in the XUV absorption spectra. By comparison to Bethe-Salpeter equation simulations, the spectral changes are mapped to real-space excited-state displacements of the lattice along the dominant A<sub>1g</sub> coordinate. By directly and simultaneously probing the excited carrier distribution dynamics and accompanying femtosecond lattice displacement in 2H-MoTe<sub>2</sub> within a single experiment, our work provides a benchmark for understanding the interplay between electronic and structural dynamics in photoexcited nanomaterials.