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

Attar, Andrew R.; Chang, Hung-Tzu; Britz, Alexander; Zhang, Xiang; Lin, Ming-Fu; Krishnamoorthy, Aravind; Linker, Thomas; Fritz, David; Neumark, Daniel M.; Kalia, Rajiv K.; Nakano, Aiichiro; Ajayan, Pulickel; Vashishta, Priya; Bergmann, Uwe; Leone, Stephen R.

doi:10.1021/acsnano.0c06988

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

Journal Article · Wed Oct 21 00:00:00 EDT 2020 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.0c06988· OSTI ID:1762184

^[1]; ^[2]; ^[1]; ^[3]; Lin, Ming-Fu ^[1]; ^[4]; Linker, Thomas ^[4]; Fritz, David ^[1]; ^[2]; Kalia, Rajiv K. ^[4]; ^[4]; ^[3]; ^[4]; ^[1]; ^[5]

SLAC National Accelerator Lab., Menlo Park, CA (United States)
Univ. of California, Berkeley, CA (United States)
Rice Univ., Houston, TX (United States)
Univ. of Southern California, Los Angeles, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

In this study, 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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: National Institutes of Health (NIH); US Air Force Office of Scientific Research (AFOSR); US Army Research Office (ARO); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; W. M. Keck Foundation

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515; SC0014607

OSTI ID:: 1762184

Alternate ID(s):: OSTI ID: 1779443

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 11 Vol. 14; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
MoTe2
carrier thermalization
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coherent lattice vibration
extreme ultraviolet pump-probe spectroscopy
transistion metal dichalcogenide

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

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