Emerging exciton physics in transition metal dichalcogenide heterobilayers

Regan, Emma C.; Wang, Danqing; Paik, Eunice Y.; Zeng, Yongxin; Zhang, Long; Zhu, Jihang; MacDonald, Allan H.; Deng, Hui; Wang, Feng

doi:10.1038/s41578-022-00440-1

Title: Emerging exciton physics in transition metal dichalcogenide heterobilayers

Abstract

Atomically thin transition metal dichalcogenides (TMDs) are 2D semiconductors with tightly bound excitons and correspondingly strong light–matter interactions. Owing to the weak van der Waals bonding between layers, TMDs can be isolated and stacked together to form synthetic heterostructures with emergent electronic and excitonic properties. In this Review, we focus on the emergent exciton physics in moiré superlattices and in TMD heterobilayers coupled to optical cavities, where exciton behaviour can be dramatically modified by the environment. Further, in moiré superlattices, a small twist angle or lattice mismatch between the layers introduces a periodic variation in the interlayer alignment that leads to exciton localization, modified optical selection rules and strong correlations. In cavity–heterostructure systems, light–matter interaction is enhanced and exciton states can couple to the cavity to form exciton-polaritons, whose properties depend on the specific TMD layers involved and their alignment. Here, we discuss recent theoretical and experimental progress towards realizing exotic exciton states in TMD heterobilayers and comment on future scientific and technological directions.

Authors:

^[1]; Wang, Danqing ^[1]; Paik, Eunice Y. ^[2];

^[3];

^[2]; Zhu, Jihang ^[3]; MacDonald, Allan H. ^[3];

^[2];

^[4]

Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Univ. of Michigan, Ann Arbor, MI (United States)
Univ. of Texas, Austin, TX (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)

Publication Date:: Wed May 04 00:00:00 EDT 2022

Research Org.:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); US Army Research Office (ARO); US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF)

OSTI Identifier:: 2329275

Grant/Contract Number:: AC02-05CH11231; W911NF-17-1-0312; FA2386-18-1-4086; DMR 1838412

Resource Type:: Accepted Manuscript

Journal Name:: Nature Reviews. Materials

Additional Journal Information:: Journal Volume: 7; Journal Issue: 10; Journal ID: ISSN 2058-8437

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Regan, Emma C., Wang, Danqing, Paik, Eunice Y., Zeng, Yongxin, Zhang, Long, Zhu, Jihang, MacDonald, Allan H., Deng, Hui, and Wang, Feng. Emerging exciton physics in transition metal dichalcogenide heterobilayers.  United States: N. p., 2022. 
Web.  doi:10.1038/s41578-022-00440-1.

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                    Regan, Emma C., Wang, Danqing, Paik, Eunice Y., Zeng, Yongxin, Zhang, Long, Zhu, Jihang, MacDonald, Allan H., Deng, Hui, & Wang, Feng. Emerging exciton physics in transition metal dichalcogenide heterobilayers.  United States.  https://doi.org/10.1038/s41578-022-00440-1

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                    Regan, Emma C., Wang, Danqing, Paik, Eunice Y., Zeng, Yongxin, Zhang, Long, Zhu, Jihang, MacDonald, Allan H., Deng, Hui, and Wang, Feng. Wed .  
"Emerging exciton physics in transition metal dichalcogenide heterobilayers".  United States.  https://doi.org/10.1038/s41578-022-00440-1.  https://www.osti.gov/servlets/purl/2329275.

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@article{osti_2329275,

  title        = {Emerging exciton physics in transition metal dichalcogenide heterobilayers},

  author       = {Regan, Emma C. and Wang, Danqing and Paik, Eunice Y. and Zeng, Yongxin and Zhang, Long and Zhu, Jihang and MacDonald, Allan H. and Deng, Hui and Wang, Feng},

  abstractNote = {Atomically thin transition metal dichalcogenides (TMDs) are 2D semiconductors with tightly bound excitons and correspondingly strong light–matter interactions. Owing to the weak van der Waals bonding between layers, TMDs can be isolated and stacked together to form synthetic heterostructures with emergent electronic and excitonic properties. In this Review, we focus on the emergent exciton physics in moiré superlattices and in TMD heterobilayers coupled to optical cavities, where exciton behaviour can be dramatically modified by the environment. Further, in moiré superlattices, a small twist angle or lattice mismatch between the layers introduces a periodic variation in the interlayer alignment that leads to exciton localization, modified optical selection rules and strong correlations. In cavity–heterostructure systems, light–matter interaction is enhanced and exciton states can couple to the cavity to form exciton-polaritons, whose properties depend on the specific TMD layers involved and their alignment. Here, we discuss recent theoretical and experimental progress towards realizing exotic exciton states in TMD heterobilayers and comment on future scientific and technological directions.},

  doi          = {10.1038/s41578-022-00440-1},

  journal      = {Nature Reviews. Materials},

  number       = 10,

  volume       = 7,

  place        = {United States},

  year         = {Wed May 04 00:00:00 EDT 2022},

  month        = {Wed May 04 00:00:00 EDT 2022}

}

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DOI: 10.1038/nnano.2012.96

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

Zeng, Hualing; Dai, Junfeng; Yao, Wang
Nature Nanotechnology, Vol. 7, Issue 8
DOI: 10.1038/nnano.2012.95

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Title: Emerging exciton physics in transition metal dichalcogenide heterobilayers

Abstract

Citation Formats

Giant Valley-Zeeman Splitting from Spin-Singlet and Spin-Triplet Interlayer Excitons in WSe 2 /MoSe 2 Heterostructure journal, December 2019

Interlayer exciton laser of extended spatial coherence in atomically thin heterostructures journal, November 2019

Breaking of Valley Degeneracy by Magnetic Field in Monolayer MoSe 2 journal, January 2015

Recent progress in the assembly of nanodevices and van der Waals heterostructures by deterministic placement of 2D materials journal, January 2018

Hubbard Model Physics in Transition Metal Dichalcogenide Moiré Bands journal, July 2018

Diffusivity Reveals Three Distinct Phases of Interlayer Excitons in MoSe 2 / WSe 2 Heterobilayers journal, March 2021

Visualizing electron localization of WS 2 /WSe 2 moiré superlattices in momentum space journal, September 2021

Measurement of the spin-forbidden dark excitons in MoS2 and MoSe2 monolayers journal, August 2020

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

2D materials and van der Waals heterostructures journal, July 2016

Anomalous Light Cones and Valley Optical Selection Rules of Interlayer Excitons in Twisted Heterobilayers journal, October 2015

van der Waals Heterostructures with High Accuracy Rotational Alignment journal, February 2016

Atomically Thin MoS2 A New Direct-Gap Semiconductor journal, September 2010

Coupling Quantum Tunneling with Cavity Photons journal, April 2012

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

Electric-field effects on exciton lifetimes in symmetric coupled GaAs/ Al 0.3 Ga 0.7 As double quantum wells journal, November 1990

Interlayer Exciton Optoelectronics in a 2D Heterostructure p–n Junction journal, January 2017

Moiré excitons: From programmable quantum emitter arrays to spin-orbit–coupled artificial lattices journal, November 2017

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

A sub-femtojoule electrical spin-switch based on optically trapped polariton condensates journal, August 2016

Experimental Evidence for Dark Excitons in Monolayer WSe 2 journal, December 2015

Cavity Control of Excitons in Two-Dimensional Materials journal, May 2019

Quantum phase transition from a superfluid to a Mott insulator in an ultracold gas of atoms journal, May 2003

Indirect Excitons and Trions in MoSe 2 /WSe 2 van der Waals Heterostructures journal, February 2020

Interactions and Magnetotransport through Spin-Valley Coupled Landau Levels in Monolayer MoS 2 journal, December 2018

Electrically Tunable Valley Dynamics in Twisted WSe 2 / WSe 2 Bilayers journal, May 2020

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

Macroscopically ordered state in an exciton system journal, August 2002

Momentum-Resolved Observation of Exciton Formation Dynamics in Monolayer WS2 journal, June 2021

Phase transition of an exciton system in GaAs coupled quantum wells journal, June 1990

Twist-angle-dependent interlayer exciton diffusion in WS2–WSe2 heterobilayers journal, May 2020

Atomic reconstruction in twisted bilayers of transition metal dichalcogenides journal, May 2020

One-Dimensional Electrical Contact to a Two-Dimensional Material journal, October 2013

Excitons in strain-induced one-dimensional moiré potentials at transition metal dichalcogenide heterojunctions journal, July 2020

Ab initio theory of moiré superlattice bands in layered two-dimensional materials journal, May 2014

Magneto-transport controlled by Landau polariton states journal, December 2018

Exciton–polaritons in van der Waals heterostructures embedded in tunable microcavities journal, October 2015

Broken mirror symmetry in excitonic response of reconstructed domains in twisted MoSe2/MoSe2 bilayers journal, July 2020

Tightly bound trions in monolayer MoS2 journal, December 2012

Twist Angle-Dependent Atomic Reconstruction and Moiré Patterns in Transition Metal Dichalcogenide Heterostructures journal, March 2020

Electrical control of interlayer exciton dynamics in atomically thin heterostructures journal, November 2019

Valley Zeeman effect in elementary optical excitations of monolayer WSe2 journal, January 2015

Bose-Einstein Condensation of Excitons journal, June 1962

Bose–Einstein condensation of excitons in bilayer electron systems journal, December 2004

Polaritons in van der Waals materials journal, October 2016

Magnetic control of valley pseudospin in monolayer WSe2 journal, January 2015

Electrically tunable topological transport of moiré polaritons journal, September 2020

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

Interlayer orientation-dependent light absorption and emission in monolayer semiconductor stacks journal, June 2015

Van der Waals heterostructure polaritons with moiré-induced nonlinearity journal, March 2021

Berezinskii-Kosterlitz-Thouless Transition in Two-Dimensional Dipole Systems journal, August 2010

Electrical tuning of optically active interlayer excitons in bilayer MoS2 journal, June 2021

Emerging Photoluminescence in Monolayer MoS2 journal, April 2010

Superconductivity and other collective phenomena in a hybrid Bose-Fermi mixture formed by a polariton condensate and an electron system in two dimensions journal, February 2016

Giant Stark splitting of an exciton in bilayer MoS2 journal, August 2020

Boson localization and the superfluid-insulator transition journal, July 1989

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

Evidence of a gate-tunable Mott insulator in a trilayer graphene moiré superlattice journal, January 2019

Signatures of moiré-trapped valley excitons in MoSe2/WSe2 heterobilayers journal, February 2019

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

Resonantly Enhanced Tunneling in a Double Layer Quantum Hall Ferromagnet journal, June 2000

Room-temperature valley coherence in a polaritonic system journal, April 2019

Excitons in a reconstructed moiré potential in twisted WSe2/WSe2 homobilayers journal, January 2021

Deep moiré potentials in twisted transition metal dichalcogenide bilayers journal, February 2021

Electrical Reservoirs for Bilayer Excitons journal, August 2018

Room-temperature exciton-polaritons with two-dimensional WS2 journal, September 2016

Twist-tailoring Coulomb correlations in van der Waals homobilayers journal, May 2020

Coulomb engineering of the bandgap and excitons in two-dimensional materials journal, May 2017

Evolution of interlayer coupling in twisted molybdenum disulfide bilayers journal, September 2014

Stripe phases in WSe2/WS2 moiré superlattices journal, March 2021

Single photon emitters in exfoliated WSe2 structures journal, May 2015

Dirac cones and Dirac saddle points of bright excitons in monolayer transition metal dichalcogenides journal, May 2014

Double Indirect Interlayer Exciton in a MoSe 2 /WSe 2 van der Waals Heterostructure journal, April 2018

Theory of two-dimensional spatially indirect equilibrium exciton condensates journal, October 2015

Controlling exciton many-body states by the electric-field effect in monolayer MoS 2 journal, April 2021

Topological Exciton Bands in Moiré Heterojunctions journal, April 2017

Spatially indirect exciton condensate phases in double bilayer graphene journal, January 2017

Giant Valley-Zeeman Splitting from Spin-Singlet and Spin-Triplet Interlayer Excitons in WSe ₂ /MoSe ₂ Heterostructure
journal, December 2019

Interlayer exciton laser of extended spatial coherence in atomically thin heterostructures
journal, November 2019

Breaking of Valley Degeneracy by Magnetic Field in Monolayer ${MoSe}_{2}$
journal, January 2015

Recent progress in the assembly of nanodevices and van der Waals heterostructures by deterministic placement of 2D materials
journal, January 2018

Hubbard Model Physics in Transition Metal Dichalcogenide Moiré Bands
journal, July 2018

Diffusivity Reveals Three Distinct Phases of Interlayer Excitons in ${MoSe}_{2} / {WSe}_{2}$ Heterobilayers
journal, March 2021

Visualizing electron localization of WS ₂ /WSe ₂ moiré superlattices in momentum space
journal, September 2021

Measurement of the spin-forbidden dark excitons in MoS2 and MoSe2 monolayers
journal, August 2020

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

2D materials and van der Waals heterostructures
journal, July 2016

Anomalous Light Cones and Valley Optical Selection Rules of Interlayer Excitons in Twisted Heterobilayers
journal, October 2015

van der Waals Heterostructures with High Accuracy Rotational Alignment
journal, February 2016

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

Coupling Quantum Tunneling with Cavity Photons
journal, April 2012

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

Electric-field effects on exciton lifetimes in symmetric coupled GaAs/ ${Al}_{0.3}$ ${Ga}_{0.7}$ As double quantum wells
journal, November 1990

Interlayer Exciton Optoelectronics in a 2D Heterostructure p–n Junction
journal, January 2017

Moiré excitons: From programmable quantum emitter arrays to spin-orbit–coupled artificial lattices
journal, November 2017

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

A sub-femtojoule electrical spin-switch based on optically trapped polariton condensates
journal, August 2016

Experimental Evidence for Dark Excitons in Monolayer ${WSe}_{2}$
journal, December 2015

Cavity Control of Excitons in Two-Dimensional Materials
journal, May 2019

Quantum phase transition from a superfluid to a Mott insulator in an ultracold gas of atoms
journal, May 2003

Indirect Excitons and Trions in MoSe ₂ /WSe ₂ van der Waals Heterostructures
journal, February 2020

Interactions and Magnetotransport through Spin-Valley Coupled Landau Levels in Monolayer ${MoS}_{2}$
journal, December 2018

Electrically Tunable Valley Dynamics in Twisted ${WSe}_{2} / {WSe}_{2}$ Bilayers
journal, May 2020

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

Macroscopically ordered state in an exciton system
journal, August 2002

Momentum-Resolved Observation of Exciton Formation Dynamics in Monolayer WS₂
journal, June 2021

Phase transition of an exciton system in GaAs coupled quantum wells
journal, June 1990

Twist-angle-dependent interlayer exciton diffusion in WS2–WSe2 heterobilayers
journal, May 2020

Atomic reconstruction in twisted bilayers of transition metal dichalcogenides
journal, May 2020

One-Dimensional Electrical Contact to a Two-Dimensional Material
journal, October 2013

Excitons in strain-induced one-dimensional moiré potentials at transition metal dichalcogenide heterojunctions
journal, July 2020

Ab initio theory of moiré superlattice bands in layered two-dimensional materials
journal, May 2014

Magneto-transport controlled by Landau polariton states
journal, December 2018

Exciton–polaritons in van der Waals heterostructures embedded in tunable microcavities
journal, October 2015

Broken mirror symmetry in excitonic response of reconstructed domains in twisted MoSe2/MoSe2 bilayers
journal, July 2020

Tightly bound trions in monolayer MoS2
journal, December 2012

Twist Angle-Dependent Atomic Reconstruction and Moiré Patterns in Transition Metal Dichalcogenide Heterostructures
journal, March 2020

Electrical control of interlayer exciton dynamics in atomically thin heterostructures
journal, November 2019

Valley Zeeman effect in elementary optical excitations of monolayer WSe2
journal, January 2015

Bose-Einstein Condensation of Excitons
journal, June 1962

Bose–Einstein condensation of excitons in bilayer electron systems
journal, December 2004

Polaritons in van der Waals materials
journal, October 2016

Magnetic control of valley pseudospin in monolayer WSe2
journal, January 2015

Electrically tunable topological transport of moiré polaritons
journal, September 2020

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

Interlayer orientation-dependent light absorption and emission in monolayer semiconductor stacks
journal, June 2015

Van der Waals heterostructure polaritons with moiré-induced nonlinearity
journal, March 2021

Berezinskii-Kosterlitz-Thouless Transition in Two-Dimensional Dipole Systems
journal, August 2010

Electrical tuning of optically active interlayer excitons in bilayer MoS2
journal, June 2021

Emerging Photoluminescence in Monolayer MoS₂
journal, April 2010

Superconductivity and other collective phenomena in a hybrid Bose-Fermi mixture formed by a polariton condensate and an electron system in two dimensions
journal, February 2016

Giant Stark splitting of an exciton in bilayer MoS2
journal, August 2020

Boson localization and the superfluid-insulator transition
journal, July 1989

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

Evidence of a gate-tunable Mott insulator in a trilayer graphene moiré superlattice
journal, January 2019

Signatures of moiré-trapped valley excitons in MoSe2/WSe2 heterobilayers
journal, February 2019

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

Resonantly Enhanced Tunneling in a Double Layer Quantum Hall Ferromagnet
journal, June 2000

Room-temperature valley coherence in a polaritonic system
journal, April 2019

Excitons in a reconstructed moiré potential in twisted WSe2/WSe2 homobilayers
journal, January 2021

Deep moiré potentials in twisted transition metal dichalcogenide bilayers
journal, February 2021

Electrical Reservoirs for Bilayer Excitons
journal, August 2018

Room-temperature exciton-polaritons with two-dimensional WS2
journal, September 2016

Twist-tailoring Coulomb correlations in van der Waals homobilayers
journal, May 2020

Coulomb engineering of the bandgap and excitons in two-dimensional materials
journal, May 2017

Evolution of interlayer coupling in twisted molybdenum disulfide bilayers
journal, September 2014

Stripe phases in WSe2/WS2 moiré superlattices
journal, March 2021

Single photon emitters in exfoliated WSe2 structures
journal, May 2015

Dirac cones and Dirac saddle points of bright excitons in monolayer transition metal dichalcogenides
journal, May 2014

Double Indirect Interlayer Exciton in a MoSe ₂ /WSe ₂ van der Waals Heterostructure
journal, April 2018

Theory of two-dimensional spatially indirect equilibrium exciton condensates
journal, October 2015

Controlling exciton many-body states by the electric-field effect in monolayer ${MoS}_{2}$
journal, April 2021

Topological Exciton Bands in Moiré Heterojunctions
journal, April 2017

Spatially indirect exciton condensate phases in double bilayer graphene
journal, January 2017

Optically active quantum dots in monolayer WSe2
journal, May 2015

Exciton-mediated superconductivity
journal, May 2016

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