Simultaneous Observation of Carrier-Specific Redistribution and Coherent Lattice Dynamics in 2H-MoTe2 with Femtosecond Core-Level Spectroscopy
Abstract
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 A1g (5.1 THz) and in-plane E1g (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 A1g 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.
- Authors:
-
[1];
[2];
[1];
[3];
[4];
[2];
[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)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; US Air Force Office of Scientific Research (AFOSR); W. M. Keck Foundation; US Army Research Office (ARO); National Institutes of Health (NIH); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1762184
- Alternate Identifier(s):
- OSTI ID: 1779443
- Grant/Contract Number:
- AC02-05CH11231; SC0014607; FA9550-14-1-0154; 046300; W911NF-14-1-0383; NIH S10OD023532; AC02-76SF00515; W911NF-14-1- 0383; FA9550-19-1-0314
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Volume: 14; Journal Issue: 11; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; transistion metal dichalcogenide; MoTe2; carrier thermalization; carrier-phonon scattering; coherent lattice vibration; extreme ultraviolet pump-probe spectroscopy
Citation Formats
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, and Leone, Stephen R. Simultaneous Observation of Carrier-Specific Redistribution and Coherent Lattice Dynamics in 2H-MoTe2 with Femtosecond Core-Level Spectroscopy. United States: N. p., 2020.
Web. doi:10.1021/acsnano.0c06988.
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. Simultaneous Observation of Carrier-Specific Redistribution and Coherent Lattice Dynamics in 2H-MoTe2 with Femtosecond Core-Level Spectroscopy. United States. https://doi.org/10.1021/acsnano.0c06988
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, and Leone, Stephen R. Wed .
"Simultaneous Observation of Carrier-Specific Redistribution and Coherent Lattice Dynamics in 2H-MoTe2 with Femtosecond Core-Level Spectroscopy". United States. https://doi.org/10.1021/acsnano.0c06988. https://www.osti.gov/servlets/purl/1762184.
@article{osti_1762184,
title = {Simultaneous Observation of Carrier-Specific Redistribution and Coherent Lattice Dynamics in 2H-MoTe2 with Femtosecond Core-Level Spectroscopy},
author = {Attar, Andrew R. and Chang, Hung-Tzu and Britz, Alexander and Zhang, Xiang and Lin, Ming-Fu and Krishnamoorthy, Aravind and Linker, Thomas and Fritz, David and Neumark, Daniel M. and Kalia, Rajiv K. and Nakano, Aiichiro and Ajayan, Pulickel and Vashishta, Priya and Bergmann, Uwe and Leone, Stephen R.},
abstractNote = {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 A1g (5.1 THz) and in-plane E1g (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 A1g 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.},
doi = {10.1021/acsnano.0c06988},
journal = {ACS Nano},
number = 11,
volume = 14,
place = {United States},
year = {Wed Oct 21 00:00:00 EDT 2020},
month = {Wed Oct 21 00:00:00 EDT 2020}
}
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