Twisted MoSe2 bilayers with variable local stacking and interlayer coupling revealed by low-frequency Raman spectroscopy

Puretzky, Alexander A.; Liang, Liangbo; Li, Xufan; Xiao, Kai; Sumpter, Bobby G.; Meunier, Vincent; Geohegan, David B.

doi:10.1021/acsnano.5b07807

Title: Twisted MoSe₂ bilayers with variable local stacking and interlayer coupling revealed by low-frequency Raman spectroscopy

Abstract

Unique twisted bilayers of MoSe₂ with multiple stacking orientations and interlayer couplings in the narrow range of twist angles, 60 ± 3°, are revealed by low-frequency Raman spectroscopy and theoretical analysis. The slight deviation from 60 allows the concomitant presence of patches featuring all three high-symmetry stacking configurations (2H or AA', AB', A'B) in one unique bilayer system. In this case, the periodic arrangement of the patches and their size strongly depend on the twist angle. Ab initio modeling predicts significant changes in frequencies and intensities of low-frequency modes versus stacking and twist angle. Experimentally, the variable stacking and coupling across the interface is revealed by the appearance of two breathing modes corresponding to the mixture of the high-symmetry stacking configurations and unaligned regions of monolayers. Only one breathing mode is observed outside the narrow range of twist angles. This indicates a stacking transition to unaligned monolayers with mismatched atom registry without the in-plane restoring force required to generate a shear mode. As a result, the variable interlayer coupling and spacing in transition metal dichalcogenide bilayers revealed in this study may provide a new platform for optoelectronic applications of these materials.

Authors:

Puretzky, Alexander A. ^[1]; Liang, Liangbo ^[1]; Li, Xufan ^[1]; Xiao, Kai ^[1]; Sumpter, Bobby G. ^[1]; Meunier, Vincent ^[2]; Geohegan, David B. ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Rensselaer Polytechnic Institute (RPI), Troy, NY (United States)

Publication Date:: Thu Jan 14 00:00:00 EST 2016

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

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1241475

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: ACS Nano

Additional Journal Information:: Journal Volume: 10; Journal Issue: 2; Journal ID: ISSN 1936-0851

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 77 NANOSCIENCE AND NANOTECHNOLOGY; two-dimensional materials; transition metal dichalcogenides; low-frequency Raman spectroscopy; stacking configurations; first-principles calculations

Citation Formats


                    Puretzky, Alexander A., Liang, Liangbo, Li, Xufan, Xiao, Kai, Sumpter, Bobby G., Meunier, Vincent, and Geohegan, David B. Twisted MoSe2 bilayers with variable local stacking and interlayer coupling revealed by low-frequency Raman spectroscopy.  United States: N. p., 2016. 
Web.  doi:10.1021/acsnano.5b07807.

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                    Puretzky, Alexander A., Liang, Liangbo, Li, Xufan, Xiao, Kai, Sumpter, Bobby G., Meunier, Vincent, & Geohegan, David B. Twisted MoSe2 bilayers with variable local stacking and interlayer coupling revealed by low-frequency Raman spectroscopy.  United States.  https://doi.org/10.1021/acsnano.5b07807

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                    Puretzky, Alexander A., Liang, Liangbo, Li, Xufan, Xiao, Kai, Sumpter, Bobby G., Meunier, Vincent, and Geohegan, David B. Thu .  
"Twisted MoSe2 bilayers with variable local stacking and interlayer coupling revealed by low-frequency Raman spectroscopy".  United States.  https://doi.org/10.1021/acsnano.5b07807.  https://www.osti.gov/servlets/purl/1241475.

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@article{osti_1241475,

  title        = {Twisted MoSe2 bilayers with variable local stacking and interlayer coupling revealed by low-frequency Raman spectroscopy},

  author       = {Puretzky, Alexander A. and Liang, Liangbo and Li, Xufan and Xiao, Kai and Sumpter, Bobby G. and Meunier, Vincent and Geohegan, David B.},

  abstractNote = {Unique twisted bilayers of MoSe2 with multiple stacking orientations and interlayer couplings in the narrow range of twist angles, 60 ± 3°, are revealed by low-frequency Raman spectroscopy and theoretical analysis. The slight deviation from 60 allows the concomitant presence of patches featuring all three high-symmetry stacking configurations (2H or AA', AB', A'B) in one unique bilayer system. In this case, the periodic arrangement of the patches and their size strongly depend on the twist angle. Ab initio modeling predicts significant changes in frequencies and intensities of low-frequency modes versus stacking and twist angle. Experimentally, the variable stacking and coupling across the interface is revealed by the appearance of two breathing modes corresponding to the mixture of the high-symmetry stacking configurations and unaligned regions of monolayers. Only one breathing mode is observed outside the narrow range of twist angles. This indicates a stacking transition to unaligned monolayers with mismatched atom registry without the in-plane restoring force required to generate a shear mode. As a result, the variable interlayer coupling and spacing in transition metal dichalcogenide bilayers revealed in this study may provide a new platform for optoelectronic applications of these materials.},

  doi          = {10.1021/acsnano.5b07807},

  journal      = {ACS Nano},

  number       = 2,

  volume       = 10,

  place        = {United States},

  year         = {Thu Jan 14 00:00:00 EST 2016},

  month        = {Thu Jan 14 00:00:00 EST 2016}

}

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Title: Twisted MoSe2 bilayers with variable local stacking and interlayer coupling revealed by low-frequency Raman spectroscopy

Abstract

Citation Formats

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

Ultrafast Charge Separation and Indirect Exciton Formation in a MoS 2 –MoSe 2 van der Waals Heterostructure journal, November 2014

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

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Probing the Interlayer Coupling of Twisted Bilayer MoS 2 Using Photoluminescence Spectroscopy journal, September 2014

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

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Recent Advances in Two-Dimensional Materials beyond Graphene journal, October 2015

Resonant Raman spectroscopy of twisted multilayer graphene journal, November 2014

The shear mode of multilayer graphene journal, February 2012

Measurement of layer breathing mode vibrations in few-layer graphene journal, March 2013

Low-Frequency Interlayer Breathing Modes in Few-Layer Black Phosphorus journal, May 2015

Large Frequency Change with Thickness in Interlayer Breathing Mode—Significant Interlayer Interactions in Few Layer Black Phosphorus journal, May 2015

Interlayer interactions in anisotropic atomically thin rhenium diselenide journal, October 2015

Enhanced ultra-low-frequency interlayer shear modes in folded graphene layers journal, August 2014

Interface Coupling in Twisted Multilayer Graphene by Resonant Raman Spectroscopy of Layer Breathing Modes journal, June 2015

Stacking sequence determines Raman intensities of observed interlayer shear modes in 2D layered materials – A general bond polarizability model journal, October 2015

Mapping of Low-Frequency Raman Modes in CVD-Grown Transition Metal Dichalcogenides: Layer Number, Stacking Orientation and Resonant Effects journal, January 2016

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

Stacking effects on the electronic and optical properties of bilayer transition metal dichalcogenides MoS 2 , MoSe 2 , WS 2 , and WSe 2 journal, February 2014

Interlayer Electronic Coupling in Arbitrarily Stacked MoS 2 Bilayers Controlled by Interlayer S–S Interaction journal, December 2014

Anharmonic properties from a generalized third-order ab initio approach: Theory and applications to graphite and graphene journal, June 2013

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

Phonons in single-layer and few-layer MoS 2 and WS 2 journal, October 2011

First-principles Raman spectra of MoS2, WS2 and their heterostructures journal, January 2014

Raman scattering intensities in α-quartz: A first-principles investigation journal, February 2001

Ab initio study of the vibrational properties of crystalline TeO 2 : The α , β , and γ phases journal, March 2006

Controlled growth of atomically thin MoSe 2 films and nanoribbons by chemical vapor deposition journal, January 2019

Raman spectroscopy of transition metal dichalcogenides journal, July 2016

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

Weakened interlayer coupling in two-dimensional MoSe2 flakes with screw dislocations journal, June 2019

Experimental and dynamical study of a dual Q-switched intracavity OPO based on few-layer MoSe 2 SA journal, January 2019

The role of collective motion in the ultrafast charge transfer in van der Waals heterostructures journal, May 2016

First principles study and empirical parametrization of twisted bilayer MoS2 based on band-unfolding journal, September 2016

Stacking-dependent interlayer phonons in 3R and 2H MoS 2 journal, February 2019

Laser Synthesis, Processing, and Spectroscopy of Atomically-Thin Two Dimensional Materials book, January 2018

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

Evolution of inter-layer coupling in artificially stacked bilayer MoS 2 journal, January 2019

Anomalous interlayer vibrations in strongly coupled layered PdSe 2 journal, May 2018

Reliable Piezoelectricity in Bilayer WSe 2 for Piezoelectric Nanogenerators journal, June 2017

Band engineering in twisted molybdenum disulfide bilayers journal, April 2018

Impact of a van der Waals interface on intrinsic and extrinsic defects in an MoSe 2 monolayer journal, August 2018

Interlayer couplings, Moiré patterns, and 2D electronic superlattices in MoS 2 /WSe 2 hetero-bilayers journal, January 2017

Isoelectronic Tungsten Doping in Monolayer MoSe 2 for Carrier Type Modulation journal, July 2016

Progress in piezotronic and piezo-phototronic effect of 2D materials journal, September 2018

Title: Twisted MoSe₂ bilayers with variable local stacking and interlayer coupling revealed by low-frequency Raman spectroscopy

Van der Waals heterostructures
journal, July 2013

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

Ultrafast Charge Separation and Indirect Exciton Formation in a MoS ₂ –MoSe ₂ van der Waals Heterostructure
journal, November 2014

Probing Interlayer Interactions in Transition Metal Dichalcogenide Heterostructures by Optical Spectroscopy: MoS ₂ /WS ₂ and MoSe ₂ /WSe ₂
journal, July 2015

Equally Efficient Interlayer Exciton Relaxation and Improved Absorption in Epitaxial and Nonepitaxial MoS ₂ /WS ₂ Heterostructures
journal, December 2014

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

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

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

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

Vertical and in-plane heterostructures from WS₂/MoS₂ monolayers
journal, September 2014

Tuning Interlayer Coupling in Large-Area Heterostructures with CVD-Grown MoS ₂ and WS ₂ Monolayers
journal, May 2014

Spectroscopic Signatures for Interlayer Coupling in MoS ₂ –WSe ₂ van der Waals Stacking
journal, August 2014

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

Probing the Interlayer Coupling of Twisted Bilayer MoS ₂ Using Photoluminescence Spectroscopy
journal, September 2014

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

Tailoring the Electronic Structure in Bilayer Molybdenum Disulfide via Interlayer Twist
journal, June 2014

Low-Frequency Raman Fingerprints of Two-Dimensional Metal Dichalcogenide Layer Stacking Configurations
journal, May 2015

Observation of interlayer phonon modes in van der Waals heterostructures
journal, April 2015

Rapid and Nondestructive Identification of Polytypism and Stacking Sequences in Few-Layer Molybdenum Diselenide by Raman Spectroscopy
journal, July 2015

Low-frequency Raman modes and electronic excitations in atomically thin MoS $_{2}$ films
journal, December 2012

Raman spectroscopy of shear and layer breathing modes in multilayer MoS $_{2}$
journal, March 2013

Interlayer Breathing and Shear Modes in Few-Trilayer MoS ₂ and WSe ₂
journal, February 2013

Phonon and Raman scattering of two-dimensional transition metal dichalcogenides from monolayer, multilayer to bulk material
journal, January 2015

Recent Advances in Two-Dimensional Materials beyond Graphene
journal, October 2015

Resonant Raman spectroscopy of twisted multilayer graphene
journal, November 2014

The shear mode of multilayer graphene
journal, February 2012

Measurement of layer breathing mode vibrations in few-layer graphene
journal, March 2013

Low-Frequency Interlayer Breathing Modes in Few-Layer Black Phosphorus
journal, May 2015

Large Frequency Change with Thickness in Interlayer Breathing Mode—Significant Interlayer Interactions in Few Layer Black Phosphorus
journal, May 2015

Interlayer interactions in anisotropic atomically thin rhenium diselenide
journal, October 2015

Enhanced ultra-low-frequency interlayer shear modes in folded graphene layers
journal, August 2014

Interface Coupling in Twisted Multilayer Graphene by Resonant Raman Spectroscopy of Layer Breathing Modes
journal, June 2015

Stacking sequence determines Raman intensities of observed interlayer shear modes in 2D layered materials – A general bond polarizability model
journal, October 2015

Mapping of Low-Frequency Raman Modes in CVD-Grown Transition Metal Dichalcogenides: Layer Number, Stacking Orientation and Resonant Effects
journal, January 2016

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

Stacking effects on the electronic and optical properties of bilayer transition metal dichalcogenides ${MoS}_{2}$ , ${MoSe}_{2}$ , ${WS}_{2}$ , and ${WSe}_{2}$
journal, February 2014

Interlayer Electronic Coupling in Arbitrarily Stacked MoS ₂ Bilayers Controlled by Interlayer S–S Interaction
journal, December 2014

Anharmonic properties from a generalized third-order ab initio approach: Theory and applications to graphite and graphene
journal, June 2013

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

Phonons in single-layer and few-layer MoS $_{2}$ and WS $_{2}$
journal, October 2011

First-principles Raman spectra of MoS2, WS2 and their heterostructures
journal, January 2014

Raman scattering intensities in α-quartz: A first-principles investigation
journal, February 2001

Ab initio study of the vibrational properties of crystalline ${TeO}_{2}$ : The $α$ , $β$ , and $γ$ phases
journal, March 2006

Controlled growth of atomically thin MoSe ₂ films and nanoribbons by chemical vapor deposition
journal, January 2019

Raman spectroscopy of transition metal dichalcogenides
journal, July 2016

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

Weakened interlayer coupling in two-dimensional MoSe2 flakes with screw dislocations
journal, June 2019

Experimental and dynamical study of a dual Q-switched intracavity OPO based on few-layer MoSe ₂ SA
journal, January 2019

The role of collective motion in the ultrafast charge transfer in van der Waals heterostructures
journal, May 2016

First principles study and empirical parametrization of twisted bilayer MoS2 based on band-unfolding
journal, September 2016

Stacking-dependent interlayer phonons in 3R and 2H MoS ₂
journal, February 2019

Laser Synthesis, Processing, and Spectroscopy of Atomically-Thin Two Dimensional Materials
book, January 2018

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

Evolution of inter-layer coupling in artificially stacked bilayer MoS ₂
journal, January 2019

Anomalous interlayer vibrations in strongly coupled layered PdSe ₂
journal, May 2018

Reliable Piezoelectricity in Bilayer WSe ₂ for Piezoelectric Nanogenerators
journal, June 2017

Band engineering in twisted molybdenum disulfide bilayers
journal, April 2018

Impact of a van der Waals interface on intrinsic and extrinsic defects in an MoSe ₂ monolayer
journal, August 2018

Interlayer couplings, Moiré patterns, and 2D electronic superlattices in MoS ₂ /WSe ₂ hetero-bilayers
journal, January 2017

Isoelectronic Tungsten Doping in Monolayer MoSe ₂ for Carrier Type Modulation
journal, July 2016

Progress in piezotronic and piezo-phototronic effect of 2D materials
journal, September 2018