Simultaneous Observation of Carrier-Specific Redistribution and Coherent Lattice Dynamics in 2H-MoTe2 with Femtosecond Core-Level Spectroscopy

被引：43

作者：

Attar, Andrew R. ^{[1
,2
]}

Chang, Hung-Tzu ^{[3
]}

Britz, Alexander ^{[1
,2
]}

Zhang, Xiang ^{[4
]}

Lin, Ming-Fu ^{[2
]}

Krishnamoorthy, Aravind ^{[5
]}

Linker, Thomas ^{[5
]}

Fritz, David ^{[2
]}

Neumark, Daniel M. ^{[3
,6
]}

Kalia, Rajiv K. ^{[5
]}

Nakano, Aiichiro ^{[5
]}

Ajayan, Pulickel ^{[4
]}

Vashishta, Priya ^{[5
]}

Bergmann, Uwe ^{[1
,2
]}

Leone, Stephen R. ^{[3
,6
,7
]}

机构：

[1] Stanford PULSE Inst, Menlo Pk, CA 94025 USA

[2] SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA 94025 USA

[3] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA

[4] Rice Univ, Dept Mat Sci & NanoEngn, Houston, TX 77005 USA

[5] Univ Southern Calif, Collab Adv Comp & Simulat, Los Angeles, CA 90089 USA

[6] Lawrence Berkeley Natl Lab, Chem Sci Div, Berkeley, CA 94720 USA

[7] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA

来源：

ACS NANO | 2020年 / 14卷 / 11期

关键词：

transition metal dichalcogenide; MoTe2; carrier thermalization; carrier-phonon scattering; coherent lattice vibration; extreme ultraviolet pump-probe spectroscopy; LAYER MOTE2; BAND-GAP; ULTRAFAST; PSEUDOPOTENTIALS; THERMALIZATION; ULTRAVIOLET; DISPLACIVE; EXCITATION; EFFICIENCY; SINGLE;

D O I：

10.1021/acsnano.0c06988

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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-MoTe2 semiconductor. By interrogating the valence electronic structure via localized Te 4d (39-46 eV) and Mo 4p (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(1g) (5.1 THz) and in-plane E-1g (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(1g) coordinate. By directly and simultaneously probing the excited carrier distribution dynamics and accompanying femtosecond lattice displacement in 2H-MoTe2 within a single experiment, our work provides a benchmark for understanding the interplay between electronic and structural dynamics in photoexcited nanomaterials.

引用

页码：15829 / 15840

页数：12

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