Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures

Rivera, Pasqual; Schaibley, John R.; Jones, Aaron M.; Ross, Jason S.; Wu, Sanfeng; Aivazian, Grant; Klement, Philip; Seyler, Kyle; Clark, Genevieve; Ghimire, Nirmal J.; Yan, Jiaqiang; Mandrus, D. G.; Yao, Wang; Xu, Xiaodong

doi:10.1038/ncomms7242

Title: Observation of long-lived interlayer excitons in monolayer MoSe₂–WSe₂ heterostructures

Abstract

Van der Waals bound heterostructures constructed with two-dimensional materials, such as graphene, boron nitride and transition metal dichalcogenides, have sparked wide interest in both device physics and technologies at the two-dimensional limit. One highly coveted heterostructure is that of differing monolayer transition metal dichalcogenides with type-II band alignment, with bound electrons and holes localized in individual monolayers, that is, interlayer excitons. Here, we report the observation of interlayer excitons in monolayer MoSe₂–WSe₂ heterostructures by photoluminescence and photoluminescence excitation spectroscopy. The energy and luminescence intensity are highly tunable by an applied vertical gate voltage. Moreover, we measure an interlayer exciton lifetime of ~1.8 ns, an order of magnitude longer than intralayer excitons in monolayers. Ultimately, our work demonstrates optical pumping of interlayer electric polarization, which may provoke further exploration of interlayer exciton condensation, as well as new applications in two-dimensional lasers, light-emitting diodes and photovoltaic devices.

Authors:

^[1]; Schaibley, John R. ^[1]; Jones, Aaron M. ^[1]; Ross, Jason S. ^[2]; Wu, Sanfeng ^[1]; Aivazian, Grant ^[1]; Klement, Philip ^[1]; Seyler, Kyle ^[1]; Clark, Genevieve ^[2]; Ghimire, Nirmal J. ^[3]; Yan, Jiaqiang ^[4]; Mandrus, D. G. ^[5]; Yao, Wang ^[6];

^[7]

Univ. of Washington, Seattle, WA (United States). Dept. of Physics
Univ. of Washington, Seattle, WA (United States). Dept. of Materials Science and Engineering
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
Univ. of Hong Kong (China). Dept. of Physics and Center of Theoretical and Computational Physics
Univ. of Washington, Seattle, WA (United States). Dept. of Physics; Univ. of Washington, Seattle, WA (United States). Dept. of Materials Science and Engineering

Publication Date:: Tue Feb 24 00:00:00 EST 2015

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Research Grant Council of Hong Kong

OSTI Identifier:: 1265431

Grant/Contract Number:: AC05-00OR22725; SC0008145; HKU705513P; HKU8/CRF/11G; DGE-0718124

Resource Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 6; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Rivera, Pasqual, Schaibley, John R., Jones, Aaron M., Ross, Jason S., Wu, Sanfeng, Aivazian, Grant, Klement, Philip, Seyler, Kyle, Clark, Genevieve, Ghimire, Nirmal J., Yan, Jiaqiang, Mandrus, D. G., Yao, Wang, and Xu, Xiaodong. Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures.  United States: N. p., 2015. 
Web.  doi:10.1038/ncomms7242.

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                    Rivera, Pasqual, Schaibley, John R., Jones, Aaron M., Ross, Jason S., Wu, Sanfeng, Aivazian, Grant, Klement, Philip, Seyler, Kyle, Clark, Genevieve, Ghimire, Nirmal J., Yan, Jiaqiang, Mandrus, D. G., Yao, Wang, & Xu, Xiaodong. Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures.  United States.  https://doi.org/10.1038/ncomms7242

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                    Rivera, Pasqual, Schaibley, John R., Jones, Aaron M., Ross, Jason S., Wu, Sanfeng, Aivazian, Grant, Klement, Philip, Seyler, Kyle, Clark, Genevieve, Ghimire, Nirmal J., Yan, Jiaqiang, Mandrus, D. G., Yao, Wang, and Xu, Xiaodong. Tue .  
"Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures".  United States.  https://doi.org/10.1038/ncomms7242.  https://www.osti.gov/servlets/purl/1265431.

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@article{osti_1265431,

  title        = {Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures},

  author       = {Rivera, Pasqual and Schaibley, John R. and Jones, Aaron M. and Ross, Jason S. and Wu, Sanfeng and Aivazian, Grant and Klement, Philip and Seyler, Kyle and Clark, Genevieve and Ghimire, Nirmal J. and Yan, Jiaqiang and Mandrus, D. G. and Yao, Wang and Xu, Xiaodong},

  abstractNote = {Van der Waals bound heterostructures constructed with two-dimensional materials, such as graphene, boron nitride and transition metal dichalcogenides, have sparked wide interest in both device physics and technologies at the two-dimensional limit. One highly coveted heterostructure is that of differing monolayer transition metal dichalcogenides with type-II band alignment, with bound electrons and holes localized in individual monolayers, that is, interlayer excitons. Here, we report the observation of interlayer excitons in monolayer MoSe2–WSe2 heterostructures by photoluminescence and photoluminescence excitation spectroscopy. The energy and luminescence intensity are highly tunable by an applied vertical gate voltage. Moreover, we measure an interlayer exciton lifetime of ~1.8 ns, an order of magnitude longer than intralayer excitons in monolayers. Ultimately, our work demonstrates optical pumping of interlayer electric polarization, which may provoke further exploration of interlayer exciton condensation, as well as new applications in two-dimensional lasers, light-emitting diodes and photovoltaic devices.},

  doi          = {10.1038/ncomms7242},

  journal      = {Nature Communications},

  number       = ,

  volume       = 6,

  place        = {United States},

  year         = {Tue Feb 24 00:00:00 EST 2015},

  month        = {Tue Feb 24 00:00:00 EST 2015}

}

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Title: Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures

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Catalysis with two-dimensional materials and their heterostructures journal, March 2016

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

Resonance Raman signature of intertube excitons in compositionally-defined carbon nanotube bundles journal, February 2018

Cross-dimensional electron-phonon coupling in van der Waals heterostructures journal, June 2019

Cavity-control of interlayer excitons in van der Waals heterostructures journal, August 2019

Repairing atomic vacancies in single-layer MoSe2 field-effect transistor and its defect dynamics journal, March 2017

Room-temperature electrical control of exciton flux in a van der Waals heterostructure journal, July 2018

Evidence for moiré excitons in van der Waals heterostructures journal, February 2019

Enhanced interlayer neutral excitons and trions in trilayer van der Waals heterostructures journal, September 2018

Interlayer exciton dynamics in van der Waals heterostructures journal, February 2019

A 2D self-assembled MoS 2 /ZnIn 2 S 4 heterostructure for efficient photocatalytic hydrogen evolution journal, January 2017

Intriguing electronic structures and optical properties of two-dimensional van der Waals heterostructures of Zr 2 CT 2 (T = O, F) with MoSe 2 and WSe 2 journal, January 2018

Electronic structure, optical and photocatalytic performance of SiC–MX 2 (M = Mo, W and X = S, Se) van der Waals heterostructures journal, January 2018

The organic–2D transition metal dichalcogenide heterointerface journal, January 2018

Enhanced exciton emission behavior and tunable band gap of ternary W(S x Se 1−x ) 2 monolayer: temperature dependent optical evidence and first-principles calculations journal, January 2018

Optoelectronic and solar cell applications of Janus monolayers and their van der Waals heterostructures journal, January 2019

Tight-binding modeling of excitonic response in van der Waals stacked 2D semiconductors journal, January 2019

Spontaneous full photocatalytic water splitting on 2D MoSe 2 /SnSe 2 and WSe 2 /SnSe 2 vdW heterostructures journal, January 2019

Physics of excitons and their transport in two dimensional transition metal dichalcogenide semiconductors journal, January 2019

Title: Observation of long-lived interlayer excitons in monolayer MoSe₂–WSe₂ heterostructures

Novel hetero-layered materials with tunable direct band gaps by sandwiching different metal disulfides and diselenides
journal, March 2013

Coupled Spin and Valley Physics in Monolayers of ${MoS}_{2}$ and Other Group-VI Dichalcogenides
journal, May 2012

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

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

Carrier and Polarization Dynamics in Monolayer ${MoS}_{2}$
journal, January 2014

Band offsets and heterostructures of two-dimensional semiconductors
journal, January 2013

Optical generation of excitonic valley coherence in monolayer WSe2
journal, August 2013

Towards Bose–Einstein condensation of excitons in potential traps
journal, May 2002

Hofstadter’s butterfly and the fractal quantum Hall effect in moiré superlattices
journal, May 2013

Emerging Photoluminescence in Monolayer MoS₂
journal, April 2010

Strong interlayer coupling in van der Waals heterostructures built from single-layer chalcogenides
journal, April 2014

Van der Waals heterostructures
journal, July 2013

Cloning of Dirac fermions in graphene superlattices
journal, May 2013

High-temperature superfluidity with indirect excitons in van der Waals heterostructures
journal, July 2014

How to make a bilayer exciton condensate flow
journal, August 2008

Electroluminescence and Photocurrent Generation from Atomically Sharp WSe ₂ /MoS ₂ Heterojunction p–n Diodes
journal, September 2014

Electronic properties of the MoS $_{2}$ -WS $_{2}$ heterojunction
journal, February 2013

Magnetoelectric effects and valley-controlled spin quantum gates in transition metal dichalcogenide bilayers
journal, June 2013

Two-dimensional atomic crystals
journal, July 2005

Ultrafast charge transfer in atomically thin MoS2/WS2 heterostructures
journal, August 2014

Massive Dirac Fermions and Hofstadter Butterfly in a van der Waals Heterostructure
journal, May 2013

Atomically Thin ${MoS}_{2}$ A New Direct-Gap Semiconductor
journal, September 2010

Tightly bound trions in monolayer MoS2
journal, December 2012

Spin–layer locking effects in optical orientation of exciton spin in bilayer WSe2
journal, January 2014

Photovoltaic Effect in an Electrically Tunable van der Waals Heterojunction
journal, July 2014

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

Electrical control of neutral and charged excitons in a monolayer semiconductor
journal, February 2013

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

Atomically thin p–n junctions with van der Waals heterointerfaces
journal, August 2014

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

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

Exciton Dynamics in Suspended Monolayer and Few-Layer MoS ₂ 2D Crystals
journal, January 2013

How to make a bilayer exciton condensate flow
text, January 2008

Two Dimensional Atomic Crystals
text, January 2005

Epitaxial Stitching and Stacking Growth of Atomically Thin Transition-Metal Dichalcogenides (TMDCs) Heterojunctions
journal, January 2017

Ultrafast Laser Spectroscopy of Two-Dimensional Materials Beyond Graphene
journal, December 2016

Interlayer Transition in a vdW Heterostructure toward Ultrahigh Detectivity Shortwave Infrared Photodetectors
journal, October 2019

Rotation-Misfit-Free Heteroepitaxial Stacking and Stitching Growth of Hexagonal Transition-Metal Dichalcogenide Monolayers by Nucleation Kinetics Controls
journal, May 2015

Lateral Built-In Potential of Monolayer MoS ₂ -WS ₂ In-Plane Heterostructures by a Shortcut Growth Strategy
journal, September 2015

2D Black Phosphorus/SrTiO ₃ -Based Programmable Photoconductive Switch
journal, July 2016

Band Structure Engineering of Interfacial Semiconductors Based on Atomically Thin Lead Iodide Crystals
journal, March 2019

Interfacial Engineering of Van der Waals Coupled 2D Layered Materials
journal, February 2017

Band Alignment of MoTe ₂ /MoS ₂ Nanocomposite Films for Enhanced Nonlinear Optical Performance
journal, January 2019

Light Emission Properties of 2D Transition Metal Dichalcogenides: Fundamentals and Applications
journal, August 2018

Lateral Bilayer MoS ₂ –WS ₂ Heterostructure Photodetectors with High Responsivity and Detectivity
journal, July 2019

Recent Progress on Exciton Polaritons in Layered Transition‐Metal Dichalcogenides
journal, September 2019

Booming Development of Group IV–VI Semiconductors: Fresh Blood of 2D Family
journal, June 2016

Tunable Control of Interlayer Excitons in WS ₂ /MoS ₂ Heterostructures via Strong Coupling with Enhanced Mie Resonances
journal, April 2019

Constructing 1D/2D heterojunction photocatalyst from FeSe ₂ nanorods and MoSe ₂ nanoplates with high photocatalytic and photoelectrochemical performance
journal, November 2019

Nonlinear optics of two‐dimensional transition metal dichalcogenides
journal, July 2019

Interlayer Excitons in Transition‐Metal Dichalcogenide Heterobilayers
journal, November 2019

Two‐Dimensional GaX/SnS ₂ ( X = S, Se) van der Waals Heterostructures for Photovoltaic Application: Heteroatom Doping Strategy to Boost Power Conversion Efficiency
journal, January 2019

Multiphonon Raman Scattering in Transition Metal Dichalcogenide Double Layers
journal, January 2020

Environmental engineering of transition metal dichalcogenide optoelectronics
journal, June 2018

Valleytronics in transition metal dichalcogenides materials
journal, August 2019

Valleytronics in 2D materials
journal, August 2016

Twinned growth behaviour of two-dimensional materials
journal, December 2016

Atomically thin resonant tunnel diodes built from synthetic van der Waals heterostructures
journal, June 2015

Catalysis with two-dimensional materials and their heterostructures
journal, March 2016

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

Resonance Raman signature of intertube excitons in compositionally-defined carbon nanotube bundles
journal, February 2018

Cross-dimensional electron-phonon coupling in van der Waals heterostructures
journal, June 2019

Cavity-control of interlayer excitons in van der Waals heterostructures
journal, August 2019

Repairing atomic vacancies in single-layer MoSe2 field-effect transistor and its defect dynamics
journal, March 2017

Room-temperature electrical control of exciton flux in a van der Waals heterostructure
journal, July 2018

Evidence for moiré excitons in van der Waals heterostructures
journal, February 2019

Enhanced interlayer neutral excitons and trions in trilayer van der Waals heterostructures
journal, September 2018

Interlayer exciton dynamics in van der Waals heterostructures
journal, February 2019

A 2D self-assembled MoS ₂ /ZnIn ₂ S ₄ heterostructure for efficient photocatalytic hydrogen evolution
journal, January 2017

Intriguing electronic structures and optical properties of two-dimensional van der Waals heterostructures of Zr ₂ CT ₂ (T = O, F) with MoSe ₂ and WSe ₂
journal, January 2018

Electronic structure, optical and photocatalytic performance of SiC–MX ₂ (M = Mo, W and X = S, Se) van der Waals heterostructures
journal, January 2018

The organic–2D transition metal dichalcogenide heterointerface
journal, January 2018

Enhanced exciton emission behavior and tunable band gap of ternary W(S _x Se _1−x ) ₂ monolayer: temperature dependent optical evidence and first-principles calculations
journal, January 2018

Optoelectronic and solar cell applications of Janus monolayers and their van der Waals heterostructures
journal, January 2019

Tight-binding modeling of excitonic response in van der Waals stacked 2D semiconductors
journal, January 2019

Spontaneous full photocatalytic water splitting on 2D MoSe ₂ /SnSe ₂ and WSe ₂ /SnSe ₂ vdW heterostructures
journal, January 2019

Physics of excitons and their transport in two dimensional transition metal dichalcogenide semiconductors
journal, January 2019

A WSe ₂ /MoSe ₂ heterostructure photovoltaic device
journal, September 2015

Materials properties of out-of-plane heterostructures of MoS ₂ -WSe ₂ and WS ₂ -MoSe ₂
journal, February 2016