Carrier-specific dynamics in 2H-MoTe2 observed by femtosecond soft x-ray absorption spectroscopy using an x-ray free-electron laser
Abstract
Femtosecond carrier dynamics in layered 2H-MoTe2 semiconductor crystals have been investigated using soft x-ray transient absorption spectroscopy at the x-ray free-electron laser (XFEL) of the Pohang Accelerator Laboratory. Following above-bandgap optical excitation of 2H-MoTe2, the photoexcited hole distribution is directly probed via short-lived transitions from the Te 3d 5/2 core level (M5-edge, 572-577 eV) to transiently unoccupied states in the valence band. The optically excited electrons are separately probed via the reduced absorption probability at the Te M5-edge involving partially occupied states of the conduction band. A 400 ± 110 fs delay is observed between this transient electron signal near the conduction band minimum compared to higher-lying states within the conduction band, which we assign to hot electron relaxation. Additionally, the transient absorption signals below and above the Te M5 edge, assigned to photoexcited holes and electrons, respectively, are observed to decay concomitantly on a 1-2 ps timescale, which is interpreted as electron-hole recombination. The present work provides a benchmark for applications of XFELs for soft x-ray absorption studies of carrier-specific dynamics in semiconductors, and future opportunities enabled by this method are discussed.
- Authors:
-
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis
- Rice Univ., Houston, TX (United States)
- Univ. of California, Berkeley, CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
- Univ. of Southern California, Los Angeles, CA (United States). Collaboratory for Advanced Computing and Simulations
- Pohang Accelerator Lab. (PAL-XFEL) (Korea, Republic of)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis; Stanford Univ., CA (United States)
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES); Stanford Univ., CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
- 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). Chemical Sciences, Geosciences & Biosciences Division; W. M. Keck Foundation; US Air Force Office of Scientific Research (AFOSR); US Army Research Office (ARO); Ministry of Education of Korea; USDOE
- OSTI Identifier:
- 1817879
- Alternate Identifier(s):
- OSTI ID: 1755665; OSTI ID: 1759111
- Grant/Contract Number:
- AC02-05CH11231; SC0014607; 2020R1A2C1007416; 2018R1D1A1B07046676; S10OD023532; 046300; A9550-19-1-0314; FA9550-14-1-0154; FA9550-15-1-0037; W911NF-14-1-0383; AC02-76SF00515; FWP 100435; DEAC02-05-CH11231; KC3103
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Structural Dynamics
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2329-7778
- Publisher:
- American Crystallographic Association/AIP
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; x-ray absorption spectroscopy; semiconductor materials; 2D materials; transition metal chalcogenides; free electron lasers; transient-absorption spectroscopy; charge recombination; femtosecond carrier dynamics; density functional theory
Citation Formats
Britz, Alexander, Attar, Andrew R., Zhang, Xiang, Chang, Hung-Tzu, Nyby, Clara, Krishnamoorthy, Aravind, Park, Sang Han, Kwon, Soonnam, Kim, Minseok, Nordlund, Dennis, Sainio, Sami, Heinz, Tony F., Leone, Stephen R., Lindenberg, Aaron M., Nakano, Aiichiro, Ajayan, Pulickel, Vashishta, Priya, Fritz, David, Lin, Ming-Fu, and Bergmann, Uwe. Carrier-specific dynamics in 2H-MoTe2 observed by femtosecond soft x-ray absorption spectroscopy using an x-ray free-electron laser. United States: N. p., 2021.
Web. doi:10.1063/4.0000048.
Britz, Alexander, Attar, Andrew R., Zhang, Xiang, Chang, Hung-Tzu, Nyby, Clara, Krishnamoorthy, Aravind, Park, Sang Han, Kwon, Soonnam, Kim, Minseok, Nordlund, Dennis, Sainio, Sami, Heinz, Tony F., Leone, Stephen R., Lindenberg, Aaron M., Nakano, Aiichiro, Ajayan, Pulickel, Vashishta, Priya, Fritz, David, Lin, Ming-Fu, & Bergmann, Uwe. Carrier-specific dynamics in 2H-MoTe2 observed by femtosecond soft x-ray absorption spectroscopy using an x-ray free-electron laser. United States. https://doi.org/10.1063/4.0000048
Britz, Alexander, Attar, Andrew R., Zhang, Xiang, Chang, Hung-Tzu, Nyby, Clara, Krishnamoorthy, Aravind, Park, Sang Han, Kwon, Soonnam, Kim, Minseok, Nordlund, Dennis, Sainio, Sami, Heinz, Tony F., Leone, Stephen R., Lindenberg, Aaron M., Nakano, Aiichiro, Ajayan, Pulickel, Vashishta, Priya, Fritz, David, Lin, Ming-Fu, and Bergmann, Uwe. Wed .
"Carrier-specific dynamics in 2H-MoTe2 observed by femtosecond soft x-ray absorption spectroscopy using an x-ray free-electron laser". United States. https://doi.org/10.1063/4.0000048. https://www.osti.gov/servlets/purl/1817879.
@article{osti_1817879,
title = {Carrier-specific dynamics in 2H-MoTe2 observed by femtosecond soft x-ray absorption spectroscopy using an x-ray free-electron laser},
author = {Britz, Alexander and Attar, Andrew R. and Zhang, Xiang and Chang, Hung-Tzu and Nyby, Clara and Krishnamoorthy, Aravind and Park, Sang Han and Kwon, Soonnam and Kim, Minseok and Nordlund, Dennis and Sainio, Sami and Heinz, Tony F. and Leone, Stephen R. and Lindenberg, Aaron M. and Nakano, Aiichiro and Ajayan, Pulickel and Vashishta, Priya and Fritz, David and Lin, Ming-Fu and Bergmann, Uwe},
abstractNote = {Femtosecond carrier dynamics in layered 2H-MoTe2 semiconductor crystals have been investigated using soft x-ray transient absorption spectroscopy at the x-ray free-electron laser (XFEL) of the Pohang Accelerator Laboratory. Following above-bandgap optical excitation of 2H-MoTe2, the photoexcited hole distribution is directly probed via short-lived transitions from the Te 3d 5/2 core level (M5-edge, 572-577 eV) to transiently unoccupied states in the valence band. The optically excited electrons are separately probed via the reduced absorption probability at the Te M5-edge involving partially occupied states of the conduction band. A 400 ± 110 fs delay is observed between this transient electron signal near the conduction band minimum compared to higher-lying states within the conduction band, which we assign to hot electron relaxation. Additionally, the transient absorption signals below and above the Te M5 edge, assigned to photoexcited holes and electrons, respectively, are observed to decay concomitantly on a 1-2 ps timescale, which is interpreted as electron-hole recombination. The present work provides a benchmark for applications of XFELs for soft x-ray absorption studies of carrier-specific dynamics in semiconductors, and future opportunities enabled by this method are discussed.},
doi = {10.1063/4.0000048},
journal = {Structural Dynamics},
number = 1,
volume = 8,
place = {United States},
year = {Wed Jan 13 00:00:00 EST 2021},
month = {Wed Jan 13 00:00:00 EST 2021}
}
Works referenced in this record:
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Femtosecond tracking of carrier relaxation in germanium with extreme ultraviolet transient reflectivity
journal, May 2018
- Kaplan, Christopher J.; Kraus, Peter M.; Ross, Andrew D.
- Physical Review B, Vol. 97, Issue 20
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Optical Properties and Band Gap of Single- and Few-Layer MoTe 2 Crystals
journal, October 2014
- Ruppert, Claudia; Aslan, Ozgur Burak; Heinz, Tony F.
- Nano Letters, Vol. 14, Issue 11
Ultrafast Spectroscopy of Semiconductors and Semiconductor Nanostructures
book, January 1999
- Shah, Jagdeep
- Springer Series in Solid-State Sciences
Carrier-Specific Femtosecond XUV Transient Absorption of PbI 2 Reveals Ultrafast Nonradiative Recombination
journal, December 2017
- Lin, Ming-Fu; Verkamp, Max A.; Leveillee, Joshua
- The Journal of Physical Chemistry C, Vol. 121, Issue 50
Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids
journal, April 2019
- Geneaux, Romain; Marroux, Hugo J. B.; Guggenmos, Alexander
- Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009
- Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
- Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
Ultrafast carrier and phonon dynamics in few-layer 2H–MoTe 2
journal, September 2019
- Chi, Zhen; Chen, Hailong; Zhao, Qing
- The Journal of Chemical Physics, Vol. 151, Issue 11
Ultrafast carrier thermalization and trapping in silicon-germanium alloy probed by extreme ultraviolet transient absorption spectroscopy
journal, July 2017
- Zürch, Michael; Chang, Hung-Tzu; Kraus, Peter M.
- Structural Dynamics, Vol. 4, Issue 4
Modulating the Functions of MoS 2 /MoTe 2 van der Waals Heterostructure via Thickness Variation
journal, March 2019
- Duong, Ngoc Thanh; Lee, Juchan; Bang, Seungho
- ACS Nano, Vol. 13, Issue 4
Time-resolved resonant elastic soft x-ray scattering at Pohang Accelerator Laboratory X-ray Free Electron Laser
journal, August 2020
- Jang, Hoyoung; Kim, Hyeong-Do; Kim, Minseok
- Review of Scientific Instruments, Vol. 91, Issue 8
Hot phonon and carrier relaxation in Si(100) determined by transient extreme ultraviolet spectroscopy
journal, September 2018
- Cushing, Scott K.; Zürch, Michael; Kraus, Peter M.
- Structural Dynamics, Vol. 5, Issue 5
Soft x-ray absorption spectroscopy of metalloproteins and high-valent metal-complexes at room temperature using free-electron lasers
journal, September 2017
- Kubin, Markus; Kern, Jan; Gul, Sheraz
- Structural Dynamics, Vol. 4, Issue 5
Ambipolar MoTe 2 Transistors and Their Applications in Logic Circuits
journal, April 2014
- Lin, Yen-Fu; Xu, Yong; Wang, Sheng-Tsung
- Advanced Materials, Vol. 26, Issue 20
A Review, Bibliography, and Tabulation of K , L , and Higher Atomic Shell X‐Ray Fluorescence Yields
journal, March 1994
- Hubbell, J. H.; Trehan, P. N.; Singh, Nirmal
- Journal of Physical and Chemical Reference Data, Vol. 23, Issue 2
Specimen charging in X-ray absorption spectroscopy: correction of total electron yield data from stabilized zirconia in the energy range 250–915 eV
journal, February 2005
- Vlachos, Dimitrios; Craven, Alan J.; McComb, David W.
- Journal of Synchrotron Radiation, Vol. 12, Issue 2
Ultrafast Carrier Thermalization and Cooling Dynamics in Few-Layer MoS 2
journal, October 2014
- Nie, Zhaogang; Long, Run; Sun, Linfeng
- ACS Nano, Vol. 8, Issue 10
Nonlinear ionic pseudopotentials in spin-density-functional calculations
journal, August 1982
- Louie, Steven G.; Froyen, Sverre; Cohen, Marvin L.
- Physical Review B, Vol. 26, Issue 4
PAL-XFEL soft X-ray scientific instruments and X-ray optics: First commissioning results
journal, May 2018
- Park, Sang Han; Kim, Minseok; Min, Changi-Ki
- Review of Scientific Instruments, Vol. 89, Issue 5
Shot-by-shot characterization of focused X-ray free electron laser pulses
journal, January 2018
- Kobayashi, Amane; Sekiguchi, Yuki; Oroguchi, Tomotaka
- Scientific Reports, Vol. 8, Issue 1
Polymorphic Layered MoTe 2 from Semiconductor, Topological Insulator, to Weyl Semimetal
journal, January 2017
- Sankar, Raman; Narsinga Rao, G.; Muthuselvam, I. Panneer
- Chemistry of Materials, Vol. 29, Issue 2
Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium
journal, June 2017
- Zürch, Michael; Chang, Hung-Tzu; Borja, Lauren J.
- Nature Communications, Vol. 8, Issue 1
Ultrafast Dynamics of Defect-Assisted Electron–Hole Recombination in Monolayer MoS 2
journal, December 2014
- Wang, Haining; Zhang, Changjian; Rana, Farhan
- Nano Letters, Vol. 15, Issue 1
Bethe-Salpeter equation calculations of core excitation spectra
journal, March 2011
- Vinson, J.; Rehr, J. J.; Kas, J. J.
- Physical Review B, Vol. 83, Issue 11
Efficient implementation of core-excitation Bethe–Salpeter equation calculations
journal, December 2015
- Gilmore, K.; Vinson, John; Shirley, E. L.
- Computer Physics Communications, Vol. 197
Direct observation of the electronic states of photoexcited hematite with ultrafast 2p3d X-ray absorption spectroscopy and resonant inelastic X-ray scattering
journal, January 2020
- Ismail, Ahmed S. M.; Uemura, Yohei; Park, Sang Han
- Physical Chemistry Chemical Physics, Vol. 22, Issue 5
Efficient pseudopotentials for plane-wave calculations
journal, January 1991
- Troullier, N.; Martins, José Luriaas
- Physical Review B, Vol. 43, Issue 3
Structural phase transition in monolayer MoTe2 driven by electrostatic doping
journal, October 2017
- Wang, Ying; Xiao, Jun; Zhu, Hanyu
- Nature, Vol. 550, Issue 7677
Low Contact Barrier in 2H/1T′ MoTe 2 In-Plane Heterostructure Synthesized by Chemical Vapor Deposition
journal, March 2019
- Zhang, Xiang; Jin, Zehua; Wang, Luqing
- ACS Applied Materials & Interfaces, Vol. 11, Issue 13
Differentiating Photoexcited Carrier and Phonon Dynamics in the Δ, L , and Γ Valleys of Si(100) with Transient Extreme Ultraviolet Spectroscopy
journal, January 2019
- Cushing, Scott K.; Lee, Angela; Porter, Ilana J.
- The Journal of Physical Chemistry C, Vol. 123, Issue 6
Phonon-Suppressed Auger Scattering of Charge Carriers in Defective Two-Dimensional Transition Metal Dichalcogenides
journal, August 2019
- Li, Linqiu; Lin, Ming-Fu; Zhang, Xiang
- Nano Letters, Vol. 19, Issue 9
Focusing of X-ray free-electron laser pulses with reflective optics
journal, December 2012
- Yumoto, Hirokatsu; Mimura, Hidekazu; Koyama, Takahisa
- Nature Photonics, Vol. 7, Issue 1
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Layer-resolved ultrafast extreme ultraviolet measurement of hole transport in a Ni-TiO 2 -Si photoanode
journal, April 2020
- Cushing, Scott K.; Porter, Ilana J.; de Roulet, Bethany R.
- Science Advances, Vol. 6, Issue 14
Ultrafast band-gap renormalization and build-up of optical gain in monolayer
journal, February 2020
- Meckbach, L.; Hader, J.; Huttner, U.
- Physical Review B, Vol. 101, Issue 7
Thickness-dependent carrier mobility of ambipolar MoTe 2 : Interplay between interface trap and Coulomb scattering
journal, May 2017
- Ji, Hyunjin; Lee, Gwanmu; Joo, Min-Kyu
- Applied Physics Letters, Vol. 110, Issue 18
Transferable relativistic Dirac-Slater pseudopotentials
journal, July 2000
- Grinberg, Ilya; Ramer, Nicholas J.; Rappe, Andrew M.
- Physical Review B, Vol. 62, Issue 4
X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92
journal, July 1993
- Henke, B. L.; Gullikson, E. M.; Davis, J. C.
- Atomic Data and Nuclear Data Tables, Vol. 54, Issue 2, p. 181-342
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Accelerated carrier recombination by grain boundary/edge defects in MBE grown transition metal dichalcogenides
journal, May 2018
- Chen, Ke; Roy, Anupam; Rai, Amritesh
- APL Materials, Vol. 6, Issue 5
Real-Time Probing of Electron Dynamics Using Attosecond Time-Resolved Spectroscopy
journal, May 2016
- Ramasesha, Krupa; Leone, Stephen R.; Neumark, Daniel M.
- Annual Review of Physical Chemistry, Vol. 67, Issue 1
Simultaneous Observation of Carrier-Specific Redistribution and Coherent Lattice Dynamics in 2H-MoTe 2 with Femtosecond Core-Level Spectroscopy
journal, October 2020
- Attar, Andrew R.; Chang, Hung-Tzu; Britz, Alexander
- ACS Nano, Vol. 14, Issue 11
Elucidating anionic oxygen activity in lithium-rich layered oxides
journal, March 2018
- Xu, Jing; Sun, Meiling; Qiao, Ruimin
- Nature Communications, Vol. 9, Issue 1
Femtosecond time-resolved X-ray absorption spectroscopy of anatase TiO2 nanoparticles using XFEL
journal, June 2017
- Obara, Yuki; Ito, Hironori; Ito, Terumasa
- Structural Dynamics, Vol. 4, Issue 4
Advanced capabilities for materials modelling with Quantum ESPRESSO
journal, October 2017
- Giannozzi, P.; Andreussi, O.; Brumme, T.
- Journal of Physics: Condensed Matter, Vol. 29, Issue 46
Field-Effect Transistors Based on Few-Layered α-MoTe 2
journal, May 2014
- Pradhan, Nihar R.; Rhodes, Daniel; Feng, Simin
- ACS Nano, Vol. 8, Issue 6
Attosecond band-gap dynamics in silicon
journal, December 2014
- Schultze, M.; Ramasesha, K.; Pemmaraju, C. D.
- Science, Vol. 346, Issue 6215
Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids
journal, April 2019
- Geneaux, Romain; Marroux, Hugo J. B.; Guggenmos, Alexander
- Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145
Real-Time Probing of Electron Dynamics Using Attosecond Time-Resolved Spectroscopy
journal, May 2016
- Ramasesha, Krupa; Leone, Stephen R.; Neumark, Daniel M.
- Annual Review of Physical Chemistry, Vol. 67, Issue 1