Valley relaxation of resident electrons and holes in a monolayer semiconductor: Dependence on carrier density and the role of substrate-induced disorder

Li, Jing; Goryca, M.; Yumigeta, K.; Li, H.; Tongay, S.; Crooker, Scott A.

doi:10.1103/physrevmaterials.5.044001

Title: Valley relaxation of resident electrons and holes in a monolayer semiconductor: Dependence on carrier density and the role of substrate-induced disorder

Abstract

Using time-resolved optical Kerr rotation, here we measure the low-temperature valley dynamics of resident electrons and holes in exfoliated ${WSe}_{2}$ monolayers as a systematic function of carrier density. In an effort to reconcile the many disparate timescales of carrier valley dynamics in monolayer semiconductors reported to date, we directly compare the doping-dependent valley relaxation in two electrostatically gated ${WSe}_{2}$ monolayers having different dielectric environments. In a fully encapsulated structure ( $hBN / {WSe}_{2} / hBN$ , where hBN is hexagonal boron nitride), valley relaxation is found to be monoexponential. The valley relaxation time $τ_{v}$ is quite long $(~ 10 μ s)$ at low carrier densities, but decreases rapidly to less than 100 ns at high electron or hole densities $≳ 2 \times 10^{12} {cm}^{- 2}$ . In contrast, in a partially encapsulated ${WSe}_{2}$ monolayer placed directly on silicon dioxide $(hBN / {WSe}_{2} / {SiO}_{2})$ , carrier valley relaxation is multiexponential at low carrier densities. The difference is attributed to environmental disorder from the ${SiO}_{2}$ substrate. Unexpectedly, very small out-of-plane magnetic fields can increase $τ_{v}$ , especially in the $hBN / {WSe}_{2} / {SiO}_{2}$ structure, suggesting that localized states induced by disorder can play an important role in depolarizing spins and mediating the valley relaxation of resident carriers in monolayer transition-metal dichalcogenide semiconductors.

Authors:

^[1]; Goryca, M. ^[1]; Yumigeta, K. ^[2]; Li, H. ^[2];

^[2];

^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States). National High Magnetic Field Lab. (MagLab)
Arizona State Univ., Tempe, AZ (United States)

Publication Date:: Mon Apr 05 00:00:00 EDT 2021

Research Org.:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF)

OSTI Identifier:: 1804434

Report Number(s):: LA-UR-21-20744
Journal ID: ISSN 2475-9953; TRN: US2212666

Grant/Contract Number:: 89233218CNA000001; SC0020653; DMR-1644779; DMR-1955889; CMMI-1933214; 1904716; 1935994; DMR-1552220

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review Materials

Additional Journal Information:: Journal Volume: 5; Journal Issue: 4; Journal ID: ISSN 2475-9953

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; high magnetic field science; valleytronics; transition-metal dichalcogenide; two-dimensional electron system

Citation Formats


                    Li, Jing, Goryca, M., Yumigeta, K., Li, H., Tongay, S., and Crooker, Scott A. Valley relaxation of resident electrons and holes in a monolayer semiconductor: Dependence on carrier density and the role of substrate-induced disorder.  United States: N. p., 2021. 
Web.  doi:10.1103/physrevmaterials.5.044001.

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                    Li, Jing, Goryca, M., Yumigeta, K., Li, H., Tongay, S., & Crooker, Scott A. Valley relaxation of resident electrons and holes in a monolayer semiconductor: Dependence on carrier density and the role of substrate-induced disorder.  United States.  https://doi.org/10.1103/physrevmaterials.5.044001

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                    Li, Jing, Goryca, M., Yumigeta, K., Li, H., Tongay, S., and Crooker, Scott A. Mon .  
"Valley relaxation of resident electrons and holes in a monolayer semiconductor: Dependence on carrier density and the role of substrate-induced disorder".  United States.  https://doi.org/10.1103/physrevmaterials.5.044001.  https://www.osti.gov/servlets/purl/1804434.

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@article{osti_1804434,

  title        = {Valley relaxation of resident electrons and holes in a monolayer semiconductor: Dependence on carrier density and the role of substrate-induced disorder},

  author       = {Li, Jing and Goryca, M. and Yumigeta, K. and Li, H. and Tongay, S. and Crooker, Scott A.},

  abstractNote = {Using time-resolved optical Kerr rotation, here we measure the low-temperature valley dynamics of resident electrons and holes in exfoliated WSe2 monolayers as a systematic function of carrier density. In an effort to reconcile the many disparate timescales of carrier valley dynamics in monolayer semiconductors reported to date, we directly compare the doping-dependent valley relaxation in two electrostatically gated WSe2 monolayers having different dielectric environments. In a fully encapsulated structure (hBN/WSe2/hBN, where hBN is hexagonal boron nitride), valley relaxation is found to be monoexponential. The valley relaxation time τv is quite long (~10μs) at low carrier densities, but decreases rapidly to less than 100 ns at high electron or hole densities ≳2×1012cm–2. In contrast, in a partially encapsulated WSe2 monolayer placed directly on silicon dioxide (hBN/WSe2/SiO2), carrier valley relaxation is multiexponential at low carrier densities. The difference is attributed to environmental disorder from the SiO2 substrate. Unexpectedly, very small out-of-plane magnetic fields can increase τv, especially in the hBN/WSe2/SiO2 structure, suggesting that localized states induced by disorder can play an important role in depolarizing spins and mediating the valley relaxation of resident carriers in monolayer transition-metal dichalcogenide semiconductors.},

  doi          = {10.1103/physrevmaterials.5.044001},

  journal      = {Physical Review Materials},

  number       = 4,

  volume       = 5,

  place        = {United States},

  year         = {Mon Apr 05 00:00:00 EDT 2021},

  month        = {Mon Apr 05 00:00:00 EDT 2021}

}

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Title: Valley relaxation of resident electrons and holes in a monolayer semiconductor: Dependence on carrier density and the role of substrate-induced disorder

Abstract

Citation Formats

Many-Body Effects in Valleytronics: Direct Measurement of Valley Lifetimes in Single-Layer MoS 2 journal, December 2013

Graphene spintronics journal, October 2014

Valley dynamics probed through charged and neutral exciton emission in monolayer WSe 2 journal, August 2014

Optically programmable electron spin memory using semiconductor quantum dots journal, November 2004

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Magnetic brightening and control of dark excitons in monolayer WSe2 journal, June 2017

Excitonic Linewidth Approaching the Homogeneous Limit in MoS 2 -Based van der Waals Heterostructures journal, May 2017

Electrical detection of spin transport in lateral ferromagnet–semiconductor devices journal, February 2007

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Valley Splitting of AlAs Two-Dimensional Electrons in a Perpendicular Magnetic Field journal, November 2002

Valley- and spin-polarized Landau levels in monolayer WSe2 journal, October 2016

Optical spin resonance and transverse spin relaxation in magnetic semiconductor quantum wells journal, September 1997

Direct measurement of exciton valley coherence in monolayer WSe2 journal, February 2016

Probing and Manipulating Valley Coherence of Dark Excitons in Monolayer WSe 2 journal, August 2019

Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide journal, September 2016

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Intervalley dark trion states with spin lifetimes of 150 ns in WSe 2 journal, June 2017

Valley-dependent optoelectronics from inversion symmetry breaking journal, June 2008

Spontaneous Valley Polarization of Interacting Carriers in a Monolayer Semiconductor journal, October 2020

Ultrafast valley relaxation dynamics in monolayer MoS 2 probed by nonequilibrium optical techniques journal, December 2015

Marrying Excitons and Plasmons in Monolayer Transition-Metal Dichalcogenides journal, November 2017

Valley-Contrasting Physics in Graphene: Magnetic Moment and Topological Transport journal, December 2007

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Long-Lived Hole Spin/Valley Polarization Probed by Kerr Rotation in Monolayer WSe 2 journal, July 2016

Long-lived nanosecond spin relaxation and spin coherence of electrons in monolayer MoS2 and WS2 journal, August 2015

First-principles method for electron-phonon coupling and electron mobility: Applications to two-dimensional materials journal, January 2016

Boron nitride substrates for high-quality graphene electronics journal, August 2010

Valley-selective circular dichroism of monolayer molybdenum disulphide journal, January 2012

Origin of spatial charge inhomogeneity in graphene journal, August 2009

Spin-valley relaxation and quantum transport regimes in two-dimensional transition-metal dichalcogenides journal, December 2014

Unveiling Valley Lifetimes of Free Charge Carriers in Monolayer WSe 2 journal, March 2020

Electron spin relaxation due to D'yakonov-Perel' and Elliot-Yafet mechanisms in monolayer MoS 2 : Role of intravalley and intervalley processes journal, March 2014

Approaching the Intrinsic Limit in Transition Metal Diselenides via Point Defect Control journal, June 2019

Light–valley interactions in 2D semiconductors journal, July 2018

Colloquium : Excitons in atomically thin transition metal dichalcogenides journal, April 2018

Exciton radiative lifetime in transition metal dichalcogenide monolayers journal, May 2016

Optically initialized robust valley-polarized holes in monolayer WSe2 journal, November 2015

Electronic measurement and control of spin transport in silicon journal, May 2007

Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers journal, July 2017

Robust optical emission polarization in MoS 2 monolayers through selective valley excitation journal, August 2012

Mode Locking of Electron Spin Coherences in Singly Charged Quantum Dots journal, July 2006

Transport Theory of Monolayer Transition-Metal Dichalcogenides through Symmetry journal, July 2013

Gate Tunable Dark Trions in Monolayer WSe 2 journal, July 2019

Spin Coherence and Dephasing of Localized Electrons in Monolayer MoS 2 journal, November 2015

Spin-phonon relaxation from a universal ab initio density-matrix approach journal, June 2020

Long-Lived Valley Polarization of Intravalley Trions in Monolayer WSe 2 journal, December 2016

Anomalous Above-Gap Photoexcitations and Optical Signatures of Localized Charge Puddles in Monolayer Molybdenum Disulfide journal, February 2017

Local Hanle-effect studies of spin drift and diffusion in n:GaAs epilayers and spin-transport devices journal, September 2007

Detection of thermodynamic “valley noise” in monolayer semiconductors: Access to intrinsic valley relaxation time scales journal, March 2019

Local Electronic Properties of Graphene on a BN Substrate via Scanning Tunneling Microscopy journal, June 2011

Encapsulation Narrows and Preserves the Excitonic Homogeneous Linewidth of Exfoliated Monolayer Mo Se 2 journal, August 2020

Ab Initio Calculations of Ultrashort Carrier Dynamics in Two-Dimensional Materials: Valley Depolarization in Single-Layer WSe 2 journal, July 2017

Dielectric disorder in two-dimensional materials journal, August 2019

Valley Polarization in Si(100) at Zero Magnetic Field journal, June 2006

Disorder in van der Waals heterostructures of 2D materials journal, May 2019

Exciton valley dynamics probed by Kerr rotation in WSe 2 monolayers journal, October 2014

Gate-Controlled Spin-Valley Locking of Resident Carriers in WSe 2 Monolayers journal, September 2017

Imaging spin dynamics in monolayer WS 2 by time-resolved Kerr rotation microscopy journal, November 2017

Valleytronics in 2D materials journal, August 2016

Observation of ultralong valley lifetime in WSe 2 /MoS 2 heterostructures journal, July 2017

Control of valley polarization in monolayer MoS2 by optical helicity journal, June 2012

Valley depolarization due to intervalley and intravalley electron-hole exchange interactions in monolayer MoS 2 journal, May 2014

Valley polarization in MoS2 monolayers by optical pumping journal, June 2012

Fine structure and lifetime of dark excitons in transition metal dichalcogenide monolayers journal, October 2017

Indirect Bandgap Puddles in Monolayer MoS 2 by Substrate-Induced Local Strain journal, September 2016

Optically programmable electron spin memory using semiconductor quantum dots journal, November 2004

Spin memory and spin-lattice relaxation in two-dimensional hexagonal crystals journal, November 2013

Defect-Induced Modification of Low-Lying Excitons and Valley Selectivity in Monolayer Transition Metal Dichalcogenides journal, October 2018

Tribomechanical Comparison between PVA Hydrogels Obtained Using Different Processing Conditions and Human Cartilage journal, October 2019

Inter-valley dark trion states with spin lifetimes of 150 ns in WSe$_2$ text, January 2017

Fine Structure and Lifetime of Dark Excitons in Transition Metal Dichalcogenide Monolayers text, January 2017

Probing and manipulating valley coherence of dark excitons in monolayer WSe$_2$ text, January 2019

Valley splitting of AlAs two-dimensional electrons in a perpendicular magnetic field text, January 2002

Electrical Detection of Spin Transport in Lateral Ferromagnet-Semiconductor Devices text, January 2007

Many-Body Effects in Valleytronics: Direct Measurement of Valley Lifetimes in Single-Layer MoS ₂
journal, December 2013

Graphene spintronics
journal, October 2014

Valley dynamics probed through charged and neutral exciton emission in monolayer ${WSe}_{2}$
journal, August 2014

Optically programmable electron spin memory using semiconductor quantum dots
journal, November 2004

Probing many-body interactions in monolayer transition-metal dichalcogenides
journal, February 2019

Tuning Valley Polarization in a ${WSe}_{2}$ Monolayer with a Tiny Magnetic Field
journal, May 2016

Valley filter and valley valve in graphene
journal, February 2007

Magnetic brightening and control of dark excitons in monolayer WSe2
journal, June 2017

Excitonic Linewidth Approaching the Homogeneous Limit in ${MoS}_{2}$ -Based van der Waals Heterostructures
journal, May 2017

Electrical detection of spin transport in lateral ferromagnet–semiconductor devices
journal, February 2007

Spin and pseudospins in layered transition metal dichalcogenides
journal, April 2014

Symmetry-forbidden intervalley scattering by atomic defects in monolayer transition-metal dichalcogenides
journal, December 2017

Valley Splitting of AlAs Two-Dimensional Electrons in a Perpendicular Magnetic Field
journal, November 2002

Valley- and spin-polarized Landau levels in monolayer WSe2
journal, October 2016

Optical spin resonance and transverse spin relaxation in magnetic semiconductor quantum wells
journal, September 1997

Direct measurement of exciton valley coherence in monolayer WSe2
journal, February 2016

Probing and Manipulating Valley Coherence of Dark Excitons in Monolayer ${WSe}_{2}$
journal, August 2019

Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide
journal, September 2016

Imaging of pure spin-valley diffusion current in WS ₂ -WSe ₂ heterostructures
journal, May 2018

Intervalley dark trion states with spin lifetimes of 150 ns in ${WSe}_{2}$
journal, June 2017

Valley-dependent optoelectronics from inversion symmetry breaking
journal, June 2008

Spontaneous Valley Polarization of Interacting Carriers in a Monolayer Semiconductor
journal, October 2020

Ultrafast valley relaxation dynamics in monolayer ${MoS}_{2}$ probed by nonequilibrium optical techniques
journal, December 2015

Marrying Excitons and Plasmons in Monolayer Transition-Metal Dichalcogenides
journal, November 2017

Valley-Contrasting Physics in Graphene: Magnetic Moment and Topological Transport
journal, December 2007

Long valley relaxation time of free carriers in monolayer ${WSe}_{2}$
journal, June 2017

Long-Lived Hole Spin/Valley Polarization Probed by Kerr Rotation in Monolayer WSe ₂
journal, July 2016

Long-lived nanosecond spin relaxation and spin coherence of electrons in monolayer MoS2 and WS2
journal, August 2015

First-principles method for electron-phonon coupling and electron mobility: Applications to two-dimensional materials
journal, January 2016

Boron nitride substrates for high-quality graphene electronics
journal, August 2010

Valley-selective circular dichroism of monolayer molybdenum disulphide
journal, January 2012

Origin of spatial charge inhomogeneity in graphene
journal, August 2009

Spin-valley relaxation and quantum transport regimes in two-dimensional transition-metal dichalcogenides
journal, December 2014

Unveiling Valley Lifetimes of Free Charge Carriers in Monolayer WSe ₂
journal, March 2020

Electron spin relaxation due to D'yakonov-Perel' and Elliot-Yafet mechanisms in monolayer ${MoS}_{2}$ : Role of intravalley and intervalley processes
journal, March 2014

Approaching the Intrinsic Limit in Transition Metal Diselenides via Point Defect Control
journal, June 2019

Light–valley interactions in 2D semiconductors
journal, July 2018

Colloquium : Excitons in atomically thin transition metal dichalcogenides
journal, April 2018

Exciton radiative lifetime in transition metal dichalcogenide monolayers
journal, May 2016

Optically initialized robust valley-polarized holes in monolayer WSe2
journal, November 2015

Electronic measurement and control of spin transport in silicon
journal, May 2007

Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers
journal, July 2017

Robust optical emission polarization in MoS $_{2}$ monolayers through selective valley excitation
journal, August 2012

Mode Locking of Electron Spin Coherences in Singly Charged Quantum Dots
journal, July 2006

Transport Theory of Monolayer Transition-Metal Dichalcogenides through Symmetry
journal, July 2013

Gate Tunable Dark Trions in Monolayer ${WSe}_{2}$
journal, July 2019

Spin Coherence and Dephasing of Localized Electrons in Monolayer MoS ₂
journal, November 2015

Spin-phonon relaxation from a universal ab initio density-matrix approach
journal, June 2020

Long-Lived Valley Polarization of Intravalley Trions in Monolayer ${WSe}_{2}$
journal, December 2016

Anomalous Above-Gap Photoexcitations and Optical Signatures of Localized Charge Puddles in Monolayer Molybdenum Disulfide
journal, February 2017

Local Hanle-effect studies of spin drift and diffusion in n:GaAs epilayers and spin-transport devices
journal, September 2007

Detection of thermodynamic “valley noise” in monolayer semiconductors: Access to intrinsic valley relaxation time scales
journal, March 2019

Local Electronic Properties of Graphene on a BN Substrate via Scanning Tunneling Microscopy
journal, June 2011

Encapsulation Narrows and Preserves the Excitonic Homogeneous Linewidth of Exfoliated Monolayer ${Mo Se}_{2}$
journal, August 2020

Ab Initio Calculations of Ultrashort Carrier Dynamics in Two-Dimensional Materials: Valley Depolarization in Single-Layer WSe ₂
journal, July 2017

Dielectric disorder in two-dimensional materials
journal, August 2019

Valley Polarization in Si(100) at Zero Magnetic Field
journal, June 2006

Disorder in van der Waals heterostructures of 2D materials
journal, May 2019

Exciton valley dynamics probed by Kerr rotation in ${WSe}_{2}$ monolayers
journal, October 2014

Gate-Controlled Spin-Valley Locking of Resident Carriers in ${WSe}_{2}$ Monolayers
journal, September 2017

Imaging spin dynamics in monolayer WS ₂ by time-resolved Kerr rotation microscopy
journal, November 2017

Valleytronics in 2D materials
journal, August 2016

Observation of ultralong valley lifetime in WSe ₂ /MoS ₂ heterostructures
journal, July 2017

Control of valley polarization in monolayer MoS2 by optical helicity
journal, June 2012

Valley depolarization due to intervalley and intravalley electron-hole exchange interactions in monolayer ${MoS}_{2}$
journal, May 2014

Valley polarization in MoS2 monolayers by optical pumping
journal, June 2012

Fine structure and lifetime of dark excitons in transition metal dichalcogenide monolayers
journal, October 2017

Indirect Bandgap Puddles in Monolayer MoS ₂ by Substrate-Induced Local Strain
journal, September 2016

Optically programmable electron spin memory using semiconductor quantum dots
journal, November 2004

Spin memory and spin-lattice relaxation in two-dimensional hexagonal crystals
journal, November 2013

Defect-Induced Modification of Low-Lying Excitons and Valley Selectivity in Monolayer Transition Metal Dichalcogenides
journal, October 2018

Tribomechanical Comparison between PVA Hydrogels Obtained Using Different Processing Conditions and Human Cartilage
journal, October 2019

Inter-valley dark trion states with spin lifetimes of 150 ns in WSe$_2$
text, January 2017

Fine Structure and Lifetime of Dark Excitons in Transition Metal Dichalcogenide Monolayers
text, January 2017

Probing and manipulating valley coherence of dark excitons in monolayer WSe$_2$
text, January 2019

Valley splitting of AlAs two-dimensional electrons in a perpendicular magnetic field
text, January 2002

Electrical Detection of Spin Transport in Lateral Ferromagnet-Semiconductor Devices
text, January 2007

Valley polarization fluctuations, bistability, and switching in two-dimensional semiconductors
journal, July 2022