Determination of band offsets, hybridization, and exciton binding in 2D semiconductor heterostructures

Wilson, Neil R.; Nguyen, Paul V.; Seyler, Kyle; Rivera, Pasqual; Marsden, Alexander J.; Laker, Zachary P. L.; Constantinescu, Gabriel C.; Kandyba, Viktor; Barinov, Alexei; Hine, Nicholas D. M.; Xu, Xiaodong; Cobden, David H.

doi:10.1126/sciadv.1601832

Title: Determination of band offsets, hybridization, and exciton binding in 2D semiconductor heterostructures

Abstract

Combining monolayers of different two-dimensional semiconductors into heterostructures creates new phenomena and device possibilities. Understanding and exploiting these phenomena hinge on knowing the electronic structure and the properties of interlayer excitations. Here, we determine the key unknown parameters in MoSe2/WSe2 heterobilayers by using rational device design and submicrometer angle-resolved photoemission spectroscopy (μ-ARPES) in combination with photoluminescence. We find that the bands in the K-point valleys are weakly hybridized, with a valence band offset of 300 meV, implying type II band alignment. We deduce that the binding energy of interlayer excitons is more than 200 meV, an order of magnitude higher than that in analogous GaAs structures. Hybridization strongly modifies the bands at Γ, but the valence band edge remains at the K points. We also find that the spectrum of a rotationally aligned heterobilayer reflects a mixture of commensurate and incommensurate domains. These results directly answer many outstanding questions about the electronic nature of MoSe2/WSe2 heterobilayers and demonstrate a practical approach for high spectral resolution in ARPES of device-scale structures.

Authors:

Wilson, Neil R. ^[1];

^[2]; Seyler, Kyle ^[2];

^[2];

^[1]; Laker, Zachary P. L. ^[1]; Constantinescu, Gabriel C. ^[3]; Kandyba, Viktor ^[4];

^[5];

^[1]; Xu, Xiaodong ^[6]; Cobden, David H. ^[2]

Univ. of Warwick, Coventry (United Kingdom). Dept. of Physics
Univ. of Washington, Seattle, WA (United States). Dept. of Physics
Univ. of Cambridge (United Kingdom). Cavendish Lab.
Elettra-Sincrotrone Trieste S.C.p.A., Trieste (Italy)
Elettra-Sincrotrone Trieste S.C.p.A., Trieste (Italy); Univ. of Trieste (Italy). Physics Dept.
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:: Wed Feb 01 00:00:00 EST 2017

Research Org.:: Univ. of Washington, Seattle, WA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1463890

Grant/Contract Number:: SC0002197; SC0008145; SC0012509

Resource Type:: Accepted Manuscript

Journal Name:: Science Advances

Additional Journal Information:: Journal Volume: 3; Journal Issue: 2; Journal ID: ISSN 2375-2548

Publisher:: AAAS

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; μ-ARPES; photoluminescence; linear-scaling DFT; 2D semiconductor; Graphene; heterobilay; erelectronic properties; band hybridization; commensuration

Citation Formats


                    Wilson, Neil R., Nguyen, Paul V., Seyler, Kyle, Rivera, Pasqual, Marsden, Alexander J., Laker, Zachary P. L., Constantinescu, Gabriel C., Kandyba, Viktor, Barinov, Alexei, Hine, Nicholas D. M., Xu, Xiaodong, and Cobden, David H. Determination of band offsets, hybridization, and exciton binding in 2D semiconductor heterostructures.  United States: N. p., 2017. 
Web.  doi:10.1126/sciadv.1601832.

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                    Wilson, Neil R., Nguyen, Paul V., Seyler, Kyle, Rivera, Pasqual, Marsden, Alexander J., Laker, Zachary P. L., Constantinescu, Gabriel C., Kandyba, Viktor, Barinov, Alexei, Hine, Nicholas D. M., Xu, Xiaodong, & Cobden, David H. Determination of band offsets, hybridization, and exciton binding in 2D semiconductor heterostructures.  United States.  https://doi.org/10.1126/sciadv.1601832

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                    Wilson, Neil R., Nguyen, Paul V., Seyler, Kyle, Rivera, Pasqual, Marsden, Alexander J., Laker, Zachary P. L., Constantinescu, Gabriel C., Kandyba, Viktor, Barinov, Alexei, Hine, Nicholas D. M., Xu, Xiaodong, and Cobden, David H. Wed .  
"Determination of band offsets, hybridization, and exciton binding in 2D semiconductor heterostructures".  United States.  https://doi.org/10.1126/sciadv.1601832.  https://www.osti.gov/servlets/purl/1463890.

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@article{osti_1463890,

  title        = {Determination of band offsets, hybridization, and exciton binding in 2D semiconductor heterostructures},

  author       = {Wilson, Neil R. and Nguyen, Paul V. and Seyler, Kyle and Rivera, Pasqual and Marsden, Alexander J. and Laker, Zachary P. L. and Constantinescu, Gabriel C. and Kandyba, Viktor and Barinov, Alexei and Hine, Nicholas D. M. and Xu, Xiaodong and Cobden, David H.},

  abstractNote = {Combining monolayers of different two-dimensional semiconductors into heterostructures creates new phenomena and device possibilities. Understanding and exploiting these phenomena hinge on knowing the electronic structure and the properties of interlayer excitations. Here, we determine the key unknown parameters in MoSe2/WSe2 heterobilayers by using rational device design and submicrometer angle-resolved photoemission spectroscopy (μ-ARPES) in combination with photoluminescence. We find that the bands in the K-point valleys are weakly hybridized, with a valence band offset of 300 meV, implying type II band alignment. We deduce that the binding energy of interlayer excitons is more than 200 meV, an order of magnitude higher than that in analogous GaAs structures. Hybridization strongly modifies the bands at Γ, but the valence band edge remains at the K points. We also find that the spectrum of a rotationally aligned heterobilayer reflects a mixture of commensurate and incommensurate domains. These results directly answer many outstanding questions about the electronic nature of MoSe2/WSe2 heterobilayers and demonstrate a practical approach for high spectral resolution in ARPES of device-scale structures.},

  doi          = {10.1126/sciadv.1601832},

  journal      = {Science Advances},

  number       = 2,

  volume       = 3,

  place        = {United States},

  year         = {Wed Feb 01 00:00:00 EST 2017},

  month        = {Wed Feb 01 00:00:00 EST 2017}

}

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Electronic structures and optical properties of realistic transition metal dichalcogenide heterostructures from first principles journal, August 2013

Probing excitonic dark states in single-layer tungsten disulphide journal, August 2014

Accurate ionic forces and geometry optimization in linear-scaling density-functional theory with local orbitals journal, May 2011

Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy journal, October 2014

Pseudopotentials periodic table: From H to Pu journal, December 2014

Introducing ONETEP : Linear-scaling density functional simulations on parallel computers journal, February 2005

Second harmonic microscopy of monolayer MoS 2 journal, April 2013

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

Probing Symmetry Properties of Few-Layer MoS 2 and h-BN by Optical Second-Harmonic Generation journal, June 2013

Direct observation of spin-polarized bulk bands in an inversion-symmetric semiconductor journal, October 2014

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

Electronic Structure of a Quasi-Freestanding MoS 2 Monolayer journal, February 2014

Observation of intense second harmonic generation from MoS 2 atomic crystals journal, May 2013

Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor journal, August 2014

Pseudopotentials for high-throughput DFT calculations journal, January 2014

Lateral heterojunctions within monolayer MoSe2–WSe2 semiconductors journal, August 2014

Light-emitting diodes by band-structure engineering in van der Waals heterostructures journal, February 2015

Direct Measurement of the Thickness-Dependent Electronic Band Structure of MoS 2 Using Angle-Resolved Photoemission Spectroscopy journal, September 2013

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

Giant Enhancement of the Optical Second-Harmonic Emission of WSe 2 Monolayers by Laser Excitation at Exciton Resonances journal, March 2015

Tightly Bound Excitons in Monolayer WSe 2 journal, July 2014

Direct observation of the transition from indirect to direct bandgap in atomically thin epitaxial MoSe2 journal, December 2013

Coexisting massive and massless Dirac fermions in symmetry-broken bilayer graphene journal, July 2013

Strong Light-Matter Interactions in Heterostructures of Atomically Thin Films journal, May 2013

Electrically tunable excitonic light-emitting diodes based on monolayer WSe2 p–n junctions journal, March 2014

Exciton Binding Energy of Monolayer WS2 journal, March 2015

Direct Observation of Interlayer Hybridization and Dirac Relativistic Carriers in Graphene/MoS 2 van der Waals Heterostructures journal, January 2015

Energy landscape and band-structure tuning in realistic MoS 2 / MoSe 2 heterostructures journal, May 2015

Fast pick up technique for high quality heterostructures of bilayer graphene and hexagonal boron nitride journal, July 2014

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

Controlling the Electronic Structure of Bilayer Graphene journal, August 2006

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

Commensurate–incommensurate transition in graphene on hexagonal boron nitride journal, April 2014

Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS 2 journal, August 2014

Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures journal, February 2015

Emergence of superlattice Dirac points in graphene on hexagonal boron nitride journal, March 2012

High Broad-Band Photoresponsivity of Mechanically Formed InSe-Graphene van der Waals Heterostructures journal, May 2015

Parallel Nanoimprint Forming of One-Dimensional Chiral Semiconductor for Strain-Engineered Optical Properties journal, August 2020

Fabrication and optical properties of semiconductor quantum wells and superlattices journal, January 1990

Excitonic devices journal, August 2017

Long-Lived Direct and Indirect Interlayer Excitons in van der Waals Heterostructures journal, August 2017

Semiconducting van der Waals Interfaces as Artificial Semiconductors journal, July 2018

Local Strain Engineering in Atomically Thin MoS 2 journal, October 2013

Origin of Indirect Optical Transitions in Few-Layer MoS 2 , WS 2 , and WSe 2 journal, October 2013

High electron mobility, quantum Hall effect and anomalous optical response in atomically thin InSe journal, November 2016

Upconverted electroluminescence via Auger scattering of interlayer excitons in van der Waals heterostructures journal, May 2019

Out-of-plane orientation of luminescent excitons in two-dimensional indium selenide journal, September 2019

Interlayer valley excitons in heterobilayers of transition metal dichalcogenides journal, August 2018

Tuning layer-hybridized moiré excitons by the quantum-confined Stark effect journal, November 2020

Polarization switching and electrical control of interlayer excitons in two-dimensional van der Waals heterostructures journal, December 2018

The direct-to-indirect band gap crossover in two-dimensional van der Waals Indium Selenide crystals journal, December 2016

Second harmonic generation in strained transition metal dichalcogenide monolayers: MoS 2 , MoSe 2 , WS 2 , and WSe 2 journal, March 2019

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

Infrared-to-violet tunable optical activity in atomic films of GaSe, InSe, and their heterostructures journal, September 2018

Magneto-optics of the spatially separated electron and hole layers in G a A s / A l x Ga 1 − x As coupled quantum wells journal, September 1999

Nobel Lecture: Quasielectric fields and band offsets: teaching electrons new tricks journal, October 2001

Twist-tailoring Coulomb correlations in van der Waals homobilayers text, January 2020

Chemical accuracy for the van der Waals density functional preprint, January 2009

Pseudopotentials for high-throughput DFT calculations text, January 2013

Electronic structures and optical properties of realistic transition metal dichalcogenide heterostructures from first principles text, January 2013

Commensurate-incommensurate transition for graphene on hexagonal boron nitride text, January 2014

Direct imaging of the band profile in single layer ${\small MoS_2}$ on graphite: quasiparticle energy gap, metallic edge states and edge band bending text, January 2014

Electroluminescence and photocurrent generation from atomically sharp WSe2/MoS2 heterojunction p-n diodes text, January 2014

Exciton Binding Energy of Monolayer WS2 text, January 2014

Probing Excitonic Dark States in Single-layer Tungsten Disulfide text, January 2014

Hybrid MPI-OpenMP Parallelism in the ONETEP Linear-Scaling Electronic Structure Code: Application to the Delamination of Cellulose Nanofibrils
journal, October 2014

Angle-resolved photoemission spectroscopy and imaging with a submicrometre probe at the SPECTROMICROSCOPY-3.2L beamline of Elettra
journal, May 2010

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

Valley-polarized exciton dynamics in a 2D semiconductor heterostructure
journal, February 2016

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

Chemical accuracy for the van der Waals density functional
journal, December 2009

Layer-dependent electronic structure of an atomically heavy two-dimensional dichalcogenide
journal, January 2015

Electronic Properties of Graphene Encapsulated with Different Two-Dimensional Atomic Crystals
journal, May 2014

k · p theory for two-dimensional transition metal dichalcogenide semiconductors
journal, April 2015

Direct Imaging of Band Profile in Single Layer MoS ₂ on Graphite: Quasiparticle Energy Gap, Metallic Edge States, and Edge Band Bending
journal, April 2014

Electronic structure, spin-orbit coupling, and interlayer interaction in bulk ${MoS}_{2}$ and ${WS}_{2}$
journal, June 2015

Determination of band alignment in the single-layer MoS2/WSe2 heterojunction
journal, July 2015

Electronic structures and optical properties of realistic transition metal dichalcogenide heterostructures from first principles
journal, August 2013

Probing excitonic dark states in single-layer tungsten disulphide
journal, August 2014

Accurate ionic forces and geometry optimization in linear-scaling density-functional theory with local orbitals
journal, May 2011

Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy
journal, October 2014

Pseudopotentials periodic table: From H to Pu
journal, December 2014

Introducing ONETEP : Linear-scaling density functional simulations on parallel computers
journal, February 2005

Second harmonic microscopy of monolayer MoS $_{2}$
journal, April 2013

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

Probing Symmetry Properties of Few-Layer MoS ₂ and h-BN by Optical Second-Harmonic Generation
journal, June 2013

Direct observation of spin-polarized bulk bands in an inversion-symmetric semiconductor
journal, October 2014

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

Electronic Structure of a Quasi-Freestanding MoS ₂ Monolayer
journal, February 2014

Observation of intense second harmonic generation from MoS $_{2}$ atomic crystals
journal, May 2013

Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
journal, August 2014

Pseudopotentials for high-throughput DFT calculations
journal, January 2014

Lateral heterojunctions within monolayer MoSe₂–WSe₂ semiconductors
journal, August 2014

Light-emitting diodes by band-structure engineering in van der Waals heterostructures
journal, February 2015

Direct Measurement of the Thickness-Dependent Electronic Band Structure of ${MoS}_{2}$ Using Angle-Resolved Photoemission Spectroscopy
journal, September 2013

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

Giant Enhancement of the Optical Second-Harmonic Emission of ${WSe}_{2}$ Monolayers by Laser Excitation at Exciton Resonances
journal, March 2015

Tightly Bound Excitons in Monolayer ${WSe}_{2}$
journal, July 2014

Direct observation of the transition from indirect to direct bandgap in atomically thin epitaxial MoSe2
journal, December 2013

Coexisting massive and massless Dirac fermions in symmetry-broken bilayer graphene
journal, July 2013

Strong Light-Matter Interactions in Heterostructures of Atomically Thin Films
journal, May 2013

Electrically tunable excitonic light-emitting diodes based on monolayer WSe2 p–n junctions
journal, March 2014

Exciton Binding Energy of Monolayer WS2
journal, March 2015

Direct Observation of Interlayer Hybridization and Dirac Relativistic Carriers in Graphene/MoS ₂ van der Waals Heterostructures
journal, January 2015

Energy landscape and band-structure tuning in realistic ${MoS}_{2} / {MoSe}_{2}$ heterostructures
journal, May 2015

Fast pick up technique for high quality heterostructures of bilayer graphene and hexagonal boron nitride
journal, July 2014

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

Controlling the Electronic Structure of Bilayer Graphene
journal, August 2006

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

Commensurate–incommensurate transition in graphene on hexagonal boron nitride
journal, April 2014

Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer ${WS}_{2}$
journal, August 2014

Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures
journal, February 2015

Emergence of superlattice Dirac points in graphene on hexagonal boron nitride
journal, March 2012

High Broad-Band Photoresponsivity of Mechanically Formed InSe-Graphene van der Waals Heterostructures
journal, May 2015

Parallel Nanoimprint Forming of One-Dimensional Chiral Semiconductor for Strain-Engineered Optical Properties
journal, August 2020

Fabrication and optical properties of semiconductor quantum wells and superlattices
journal, January 1990

Excitonic devices
journal, August 2017

Long-Lived Direct and Indirect Interlayer Excitons in van der Waals Heterostructures
journal, August 2017

Semiconducting van der Waals Interfaces as Artificial Semiconductors
journal, July 2018

Local Strain Engineering in Atomically Thin MoS ₂
journal, October 2013

Origin of Indirect Optical Transitions in Few-Layer MoS ₂ , WS ₂ , and WSe ₂
journal, October 2013

High electron mobility, quantum Hall effect and anomalous optical response in atomically thin InSe
journal, November 2016

Upconverted electroluminescence via Auger scattering of interlayer excitons in van der Waals heterostructures
journal, May 2019

Out-of-plane orientation of luminescent excitons in two-dimensional indium selenide
journal, September 2019

Interlayer valley excitons in heterobilayers of transition metal dichalcogenides
journal, August 2018

Tuning layer-hybridized moiré excitons by the quantum-confined Stark effect
journal, November 2020

Polarization switching and electrical control of interlayer excitons in two-dimensional van der Waals heterostructures
journal, December 2018

The direct-to-indirect band gap crossover in two-dimensional van der Waals Indium Selenide crystals
journal, December 2016

Second harmonic generation in strained transition metal dichalcogenide monolayers: MoS ₂ , MoSe ₂ , WS ₂ , and WSe ₂
journal, March 2019

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

Infrared-to-violet tunable optical activity in atomic films of GaSe, InSe, and their heterostructures
journal, September 2018

Magneto-optics of the spatially separated electron and hole layers in ${G a A s / A l}_{x} {Ga}_{1 - x} As$ coupled quantum wells
journal, September 1999

Nobel Lecture: Quasielectric fields and band offsets: teaching electrons new tricks
journal, October 2001

Twist-tailoring Coulomb correlations in van der Waals homobilayers
text, January 2020

Chemical accuracy for the van der Waals density functional
preprint, January 2009

Pseudopotentials for high-throughput DFT calculations
text, January 2013

Electronic structures and optical properties of realistic transition metal dichalcogenide heterostructures from first principles
text, January 2013

Commensurate-incommensurate transition for graphene on hexagonal boron nitride
text, January 2014

Direct imaging of the band profile in single layer ${\small MoS_2}$ on graphite: quasiparticle energy gap, metallic edge states and edge band bending
text, January 2014

Electroluminescence and photocurrent generation from atomically sharp WSe2/MoS2 heterojunction p-n diodes
text, January 2014

Exciton Binding Energy of Monolayer WS2
text, January 2014

Probing Excitonic Dark States in Single-layer Tungsten Disulfide
text, January 2014

k.p theory for two-dimensional transition metal dichalcogenide semiconductors
text, January 2014

Light-emitting diodes by bandstructure engineering in van der Waals heterostructures
text, January 2014

Anomalous light cones and valley optical selection rules of interlayer excitons in twisted heterobilayers
text, January 2015