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Title: Carrier and Phonon Dynamics in Multilayer WSe2 Captured by Extreme Ultraviolet Transient Absorption Spectroscopy

Abstract

Carrier and phonon dynamics in a multilayer WSe2 film are captured by extreme ultraviolet (XUV) transient absorption (TA) spectroscopy at the W N6,7, W O2,3, and Se M4,5 edges (30–60 eV). After the broadband optical pump pulse, the XUV probe directly reports on occupations of optically excited holes and phonon-induced band renormalizations. Here, when compared with density functional theory calculations, XUV transient absorption due to holes is identified below the W O3 edge whereas signals at the Se M4,5 edges are dominated by phonon dynamics. Therein, 0.4 ps hole relaxation time, 1.5 ps carrier recombination time, and 1.7 ps phonon heating time are extracted. The acquisition of hole and phonon-induced signals in a single experiment can facilitate the investigation of the correlations between electron and phonon dynamics. Furthermore, the simultaneous observation of signals from different elements can be further extended to explore photochemical processes in multilayers and alloys, thereby providing key information for their applications in electronics, photocatalysts, and spintronics.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [3];  [3]; ORCiD logo [4]
  1. Univ. of California, Berkeley, CA (United States); Soonchunhyang Univ., Asan (Korea, Republic of)
  2. Univ. of California, Berkeley, CA (United States); Max Planck Institute for Multidisciplinary Sciences, Gottingen (Germany)
  3. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
  4. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry; Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); US Air Force Office of Scientific Research (AFOSR); Defense Advanced Research Projects Agency (DARPA); US Army Research Office (ARO)
OSTI Identifier:
2234156
Grant/Contract Number:  
AC02-05CH11231; FA9550-19-1-0314; FA9550-20-1-0334; FA9550-15-0037; FA9550-14-1-0154; W31P4Q-13-1-0017; W911NF-14-1-0383
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 127; Journal Issue: 10; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; absorption; carrier dynamics; energy; light absorption; phonons

Citation Formats

Oh, Juwon, Chang, Hung-Tzu, Chen, Christopher T., Aloni, Shaul, Schwartzberg, Adam, and Leone, Stephen R. Carrier and Phonon Dynamics in Multilayer WSe2 Captured by Extreme Ultraviolet Transient Absorption Spectroscopy. United States: N. p., 2023. Web. doi:10.1021/acs.jpcc.2c07695.
Oh, Juwon, Chang, Hung-Tzu, Chen, Christopher T., Aloni, Shaul, Schwartzberg, Adam, & Leone, Stephen R. Carrier and Phonon Dynamics in Multilayer WSe2 Captured by Extreme Ultraviolet Transient Absorption Spectroscopy. United States. https://doi.org/10.1021/acs.jpcc.2c07695
Oh, Juwon, Chang, Hung-Tzu, Chen, Christopher T., Aloni, Shaul, Schwartzberg, Adam, and Leone, Stephen R. Wed . "Carrier and Phonon Dynamics in Multilayer WSe2 Captured by Extreme Ultraviolet Transient Absorption Spectroscopy". United States. https://doi.org/10.1021/acs.jpcc.2c07695. https://www.osti.gov/servlets/purl/2234156.
@article{osti_2234156,
title = {Carrier and Phonon Dynamics in Multilayer WSe2 Captured by Extreme Ultraviolet Transient Absorption Spectroscopy},
author = {Oh, Juwon and Chang, Hung-Tzu and Chen, Christopher T. and Aloni, Shaul and Schwartzberg, Adam and Leone, Stephen R.},
abstractNote = {Carrier and phonon dynamics in a multilayer WSe2 film are captured by extreme ultraviolet (XUV) transient absorption (TA) spectroscopy at the W N6,7, W O2,3, and Se M4,5 edges (30–60 eV). After the broadband optical pump pulse, the XUV probe directly reports on occupations of optically excited holes and phonon-induced band renormalizations. Here, when compared with density functional theory calculations, XUV transient absorption due to holes is identified below the W O3 edge whereas signals at the Se M4,5 edges are dominated by phonon dynamics. Therein, 0.4 ps hole relaxation time, 1.5 ps carrier recombination time, and 1.7 ps phonon heating time are extracted. The acquisition of hole and phonon-induced signals in a single experiment can facilitate the investigation of the correlations between electron and phonon dynamics. Furthermore, the simultaneous observation of signals from different elements can be further extended to explore photochemical processes in multilayers and alloys, thereby providing key information for their applications in electronics, photocatalysts, and spintronics.},
doi = {10.1021/acs.jpcc.2c07695},
journal = {Journal of Physical Chemistry. C},
number = 10,
volume = 127,
place = {United States},
year = {Wed Mar 01 00:00:00 EST 2023},
month = {Wed Mar 01 00:00:00 EST 2023}
}

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