Carrier-specific dynamics in 2H-MoTe2 observed by femtosecond soft x-ray absorption spectroscopy using an x-ray free-electron laser

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

doi:10.1063/4.0000048

Title: 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:

^[1];

^[2]; Zhang, Xiang ^[3];

^[4];

^[5]; Krishnamoorthy, Aravind ^[6];

^[7];

^[7]; Kim, Minseok ^[7]; Nordlund, Dennis ^[8];

^[8];

^[9];

^[10]; Lindenberg, Aaron M. ^[11];

^[6]; Ajayan, Pulickel ^[3]; Vashishta, Priya ^[6]; Fritz, David ^[12];

^[12];

^[13]

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:: Wed Jan 13 00:00:00 EST 2021

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.

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                    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

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                    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.

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@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}

}

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Title: Carrier-specific dynamics in 2H-MoTe2 observed by femtosecond soft x-ray absorption spectroscopy using an x-ray free-electron laser

Abstract

Citation Formats

Generalized Gradient Approximation Made Simple journal, October 1996

Femtosecond tracking of carrier relaxation in germanium with extreme ultraviolet transient reflectivity journal, May 2018

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Optical Properties and Band Gap of Single- and Few-Layer MoTe 2 Crystals journal, October 2014

Ultrafast Spectroscopy of Semiconductors and Semiconductor Nanostructures book, January 1999

NEXAFS Spectroscopy book, January 1992

Carrier-Specific Femtosecond XUV Transient Absorption of PbI 2 Reveals Ultrafast Nonradiative Recombination journal, December 2017

Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids journal, April 2019

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials journal, September 2009

Ultrafast carrier and phonon dynamics in few-layer 2H–MoTe 2 journal, September 2019

Ultrafast carrier thermalization and trapping in silicon-germanium alloy probed by extreme ultraviolet transient absorption spectroscopy journal, July 2017

Modulating the Functions of MoS 2 /MoTe 2 van der Waals Heterostructure via Thickness Variation journal, March 2019

Time-resolved resonant elastic soft x-ray scattering at Pohang Accelerator Laboratory X-ray Free Electron Laser journal, August 2020

Hot phonon and carrier relaxation in Si(100) determined by transient extreme ultraviolet spectroscopy journal, September 2018

Soft x-ray absorption spectroscopy of metalloproteins and high-valent metal-complexes at room temperature using free-electron lasers journal, September 2017

Ambipolar MoTe 2 Transistors and Their Applications in Logic Circuits journal, April 2014

A Review, Bibliography, and Tabulation of K , L , and Higher Atomic Shell X‐Ray Fluorescence Yields journal, March 1994

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

Ultrafast Carrier Thermalization and Cooling Dynamics in Few-Layer MoS 2 journal, October 2014

Nonlinear ionic pseudopotentials in spin-density-functional calculations journal, August 1982

PAL-XFEL soft X-ray scientific instruments and X-ray optics: First commissioning results journal, May 2018

Shot-by-shot characterization of focused X-ray free electron laser pulses journal, January 2018

Polymorphic Layered MoTe 2 from Semiconductor, Topological Insulator, to Weyl Semimetal journal, January 2017

Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium journal, June 2017

Ultrafast Dynamics of Defect-Assisted Electron–Hole Recombination in Monolayer MoS 2 journal, December 2014

Bethe-Salpeter equation calculations of core excitation spectra journal, March 2011

Efficient implementation of core-excitation Bethe–Salpeter equation calculations journal, December 2015

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

Efficient pseudopotentials for plane-wave calculations journal, January 1991

Structural phase transition in monolayer MoTe2 driven by electrostatic doping journal, October 2017

Low Contact Barrier in 2H/1T′ MoTe 2 In-Plane Heterostructure Synthesized by Chemical Vapor Deposition journal, March 2019

Differentiating Photoexcited Carrier and Phonon Dynamics in the Δ, L , and Γ Valleys of Si(100) with Transient Extreme Ultraviolet Spectroscopy journal, January 2019

Phonon-Suppressed Auger Scattering of Charge Carriers in Defective Two-Dimensional Transition Metal Dichalcogenides journal, August 2019

Focusing of X-ray free-electron laser pulses with reflective optics journal, December 2012

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal, July 1996

Layer-resolved ultrafast extreme ultraviolet measurement of hole transport in a Ni-TiO 2 -Si photoanode journal, April 2020

Ultrafast band-gap renormalization and build-up of optical gain in monolayer MoTe 2 journal, February 2020

Thickness-dependent carrier mobility of ambipolar MoTe 2 : Interplay between interface trap and Coulomb scattering journal, May 2017

Transferable relativistic Dirac-Slater pseudopotentials journal, July 2000

X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92 journal, July 1993

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal, October 1996

Accelerated carrier recombination by grain boundary/edge defects in MBE grown transition metal dichalcogenides journal, May 2018

Real-Time Probing of Electron Dynamics Using Attosecond Time-Resolved Spectroscopy journal, May 2016

Simultaneous Observation of Carrier-Specific Redistribution and Coherent Lattice Dynamics in 2H-MoTe 2 with Femtosecond Core-Level Spectroscopy journal, October 2020

Elucidating anionic oxygen activity in lithium-rich layered oxides journal, March 2018

Femtosecond time-resolved X-ray absorption spectroscopy of anatase TiO2 nanoparticles using XFEL journal, June 2017

Advanced capabilities for materials modelling with Quantum ESPRESSO journal, October 2017

Field-Effect Transistors Based on Few-Layered α-MoTe 2 journal, May 2014

Attosecond band-gap dynamics in silicon journal, December 2014

Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids journal, April 2019

Real-Time Probing of Electron Dynamics Using Attosecond Time-Resolved Spectroscopy journal, May 2016

Title: Carrier-specific dynamics in 2H-MoTe₂ observed by femtosecond soft x-ray absorption spectroscopy using an x-ray free-electron laser

Generalized Gradient Approximation Made Simple
journal, October 1996

Femtosecond tracking of carrier relaxation in germanium with extreme ultraviolet transient reflectivity
journal, May 2018

Projector augmented-wave method
journal, December 1994

Optical Properties and Band Gap of Single- and Few-Layer MoTe ₂ Crystals
journal, October 2014

Ultrafast Spectroscopy of Semiconductors and Semiconductor Nanostructures
book, January 1999

NEXAFS Spectroscopy
book, January 1992

Carrier-Specific Femtosecond XUV Transient Absorption of PbI ₂ Reveals Ultrafast Nonradiative Recombination
journal, December 2017

Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids
journal, April 2019

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

Ultrafast carrier and phonon dynamics in few-layer 2H–MoTe ₂
journal, September 2019

Ultrafast carrier thermalization and trapping in silicon-germanium alloy probed by extreme ultraviolet transient absorption spectroscopy
journal, July 2017

Modulating the Functions of MoS ₂ /MoTe ₂ van der Waals Heterostructure via Thickness Variation
journal, March 2019

Time-resolved resonant elastic soft x-ray scattering at Pohang Accelerator Laboratory X-ray Free Electron Laser
journal, August 2020

Hot phonon and carrier relaxation in Si(100) determined by transient extreme ultraviolet spectroscopy
journal, September 2018

Soft x-ray absorption spectroscopy of metalloproteins and high-valent metal-complexes at room temperature using free-electron lasers
journal, September 2017

Ambipolar MoTe ₂ Transistors and Their Applications in Logic Circuits
journal, April 2014

A Review, Bibliography, and Tabulation of K , L , and Higher Atomic Shell X‐Ray Fluorescence Yields
journal, March 1994

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

Ultrafast Carrier Thermalization and Cooling Dynamics in Few-Layer MoS ₂
journal, October 2014

Nonlinear ionic pseudopotentials in spin-density-functional calculations
journal, August 1982

PAL-XFEL soft X-ray scientific instruments and X-ray optics: First commissioning results
journal, May 2018

Shot-by-shot characterization of focused X-ray free electron laser pulses
journal, January 2018

Polymorphic Layered MoTe ₂ from Semiconductor, Topological Insulator, to Weyl Semimetal
journal, January 2017

Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium
journal, June 2017

Ultrafast Dynamics of Defect-Assisted Electron–Hole Recombination in Monolayer MoS ₂
journal, December 2014

Bethe-Salpeter equation calculations of core excitation spectra
journal, March 2011

Efficient implementation of core-excitation Bethe–Salpeter equation calculations
journal, December 2015

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

Efficient pseudopotentials for plane-wave calculations
journal, January 1991

Structural phase transition in monolayer MoTe2 driven by electrostatic doping
journal, October 2017

Low Contact Barrier in 2H/1T′ MoTe ₂ In-Plane Heterostructure Synthesized by Chemical Vapor Deposition
journal, March 2019

Differentiating Photoexcited Carrier and Phonon Dynamics in the Δ, L , and Γ Valleys of Si(100) with Transient Extreme Ultraviolet Spectroscopy
journal, January 2019

Phonon-Suppressed Auger Scattering of Charge Carriers in Defective Two-Dimensional Transition Metal Dichalcogenides
journal, August 2019

Focusing of X-ray free-electron laser pulses with reflective optics
journal, December 2012

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Layer-resolved ultrafast extreme ultraviolet measurement of hole transport in a Ni-TiO ₂ -Si photoanode
journal, April 2020

Ultrafast band-gap renormalization and build-up of optical gain in monolayer ${MoTe}_{2}$
journal, February 2020

Thickness-dependent carrier mobility of ambipolar MoTe ₂ : Interplay between interface trap and Coulomb scattering
journal, May 2017

Transferable relativistic Dirac-Slater pseudopotentials
journal, July 2000

X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92
journal, July 1993

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Accelerated carrier recombination by grain boundary/edge defects in MBE grown transition metal dichalcogenides
journal, May 2018

Real-Time Probing of Electron Dynamics Using Attosecond Time-Resolved Spectroscopy
journal, May 2016

Simultaneous Observation of Carrier-Specific Redistribution and Coherent Lattice Dynamics in 2H-MoTe ₂ with Femtosecond Core-Level Spectroscopy
journal, October 2020

Elucidating anionic oxygen activity in lithium-rich layered oxides
journal, March 2018

Femtosecond time-resolved X-ray absorption spectroscopy of anatase TiO2 nanoparticles using XFEL
journal, June 2017

Advanced capabilities for materials modelling with Quantum ESPRESSO
journal, October 2017

Field-Effect Transistors Based on Few-Layered α-MoTe ₂
journal, May 2014

Attosecond band-gap dynamics in silicon
journal, December 2014

Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids
journal, April 2019

Real-Time Probing of Electron Dynamics Using Attosecond Time-Resolved Spectroscopy
journal, May 2016