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Title: Evolution of interlayer coupling in twisted molybdenum disulfide bilayers

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms5966· OSTI ID:1494115
 [1];  [2];  [3];  [2];  [3];  [4];  [3];  [3];  [3];  [3]
  1. Univ. of California, Berkeley, CA (United States); Peking Univ., Beijing (China)
  2. Univ. of California, Berkeley, CA (United States)
  3. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Van der Waals (vdW) coupling is emerging as a powerful method to engineer and tailor physical properties of atomically thin two-dimensional (2D) materials. In graphene/graphene and graphene/boron-nitride structures it leads to interesting physical phenomena ranging from new van Hove singularities and Fermi velocity renormalization to unconventional quantum Hall effects and Hofstadter's butterfly pattern. 2D transition metal dichalcogenides (TMDCs), another system of predominantly vdW-coupled atomically thin layers can also exhibit interesting but different coupling phenomena because TMDCs can be direct or indirect bandgap semiconductors. Here, we present the first study on the evolution of interlayer coupling with twist angles in as-grown MoS2 bilayers. We find that an indirect bandgap emerges in bilayers with any stacking configuration, but the bandgap size varies appreciably with the twist angle: it shows the largest redshift for AA- and AB-stacked bilayers, and a significantly smaller but constant redshift for all other twist angles. The vibration frequency of the out-of-plane phonon in MoS2 shows similar twist angle dependence. Furthermore, our observations, together with ab initio calculations, reveal that this evolution of interlayer coupling originates from the repulsive steric effects, which leads to different interlayer separations between the two MoS2 layers in different stacking configurations.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1494115
Journal Information:
Nature Communications, Vol. 5, Issue 1; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 486 works
Citation information provided by
Web of Science

References (39)

Observation of Van Hove singularities in twisted graphene layers journal November 2009
Emergence of superlattice Dirac points in graphene on hexagonal boron nitride journal March 2012
Raman Spectroscopy Study of Rotated Double-Layer Graphene: Misorientation-Angle Dependence of Electronic Structure journal June 2012
Angle-Resolved Raman Imaging of Interlayer Rotations and Interactions in Twisted Bilayer Graphene journal May 2012
Localization of Dirac Electrons in Rotated Graphene Bilayers journal March 2010
Single-Layer Behavior and Its Breakdown in Twisted Graphene Layers journal March 2011
Unconventional quantum Hall effect and Berry’s phase of 2π in bilayer graphene journal February 2006
Energy levels and wave functions of Bloch electrons in rational and irrational magnetic fields journal September 1976
Moire bands in twisted double-layer graphene journal July 2011
Hofstadter’s butterfly and the fractal quantum Hall effect in moiré superlattices journal May 2013
Massive Dirac Fermions and Hofstadter Butterfly in a van der Waals Heterostructure journal May 2013
Cloning of Dirac fermions in graphene superlattices journal May 2013
Electronics and optoelectronics of two-dimensional transition metal dichalcogenides journal November 2012
Van der Waals heterostructures journal July 2013
Atomically Thin MoS2 A New Direct-Gap Semiconductor journal September 2010
Emerging Photoluminescence in Monolayer MoS2 journal April 2010
Optical Spectrum of MoS 2 : Many-Body Effects and Diversity of Exciton States journal November 2013
Valley-selective circular dichroism of monolayer molybdenum disulphide journal January 2012
Control of valley polarization in monolayer MoS2 by optical helicity journal June 2012
Valley polarization in MoS2 monolayers by optical pumping journal June 2012
Single-layer MoS2 transistors journal January 2011
Ultrasensitive photodetectors based on monolayer MoS2 journal June 2013
Strain-engineered artificial atom as a broad-spectrum solar energy funnel journal November 2012
Electrical tuning of valley magnetic moment through symmetry control in bilayer MoS2 journal January 2013
Zeeman-type spin splitting controlled by an electric field journal July 2013
Synthesis of Large-Area MoS2 Atomic Layers with Chemical Vapor Deposition journal March 2012
Vapour phase growth and grain boundary structure of molybdenum disulphide atomic layers journal June 2013
Grains and grain boundaries in highly crystalline monolayer molybdenum disulphide journal May 2013
Size-dependent structure of MoS2 nanocrystals journal January 2007
One-Dimensional Metallic Edge States in MoS 2 journal October 2001
Probing Symmetry Properties of Few-Layer MoS 2 and h-BN by Optical Second-Harmonic Generation journal June 2013
Anomalous Lattice Vibrations of Single- and Few-Layer MoS 2 journal March 2010
Phonons in single-layer and few-layer MoS 2 and WS 2 journal October 2011
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials journal September 2009
One-Dimensional Metallic Edge States in MoS2 text January 2001
Anomalous Lattice Vibrations of Single and Few-Layer MoS2 text January 2010
Moire bands in twisted double-layer graphene text January 2010
Cloning of Dirac fermions in graphene superlattices text January 2012
Unconventional quantum Hall effect and Berry's phase of 2pi in bilayer graphene text January 2006

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Observation of Strong Interlayer Coupling in MoS 2 /WS 2 Heterostructures journal December 2015
Vertically Conductive MoS 2 Spiral Pyramid journal June 2016
High-Mobility Multilayered MoS 2 Flakes with Low Contact Resistance Grown by Chemical Vapor Deposition journal February 2017
Superlubricity between MoS 2 Monolayers journal May 2017
Nonlinear Optics with 2D Layered Materials journal March 2018
Interface Characterization and Control of 2D Materials and Heterostructures journal July 2018
Healing of Planar Defects in 2D Materials via Grain Boundary Sliding journal February 2019
Interfacial Engineering of Van der Waals Coupled 2D Layered Materials journal February 2017
Luminescence in 2D Materials and van der Waals Heterostructures journal March 2018
Photoexcitation in Solids: First-Principles Quantum Simulations by Real-Time TDDFT journal July 2018
A First‐Principles Study of Electronic Properties of Twisted MoTe 2 journal September 2019
Alpha Lead Oxide (α-PbO): A New 2D Material with Visible Light Sensitivity journal February 2018
Atomic‐Scale Fabrication of In‐Plane Heterojunctions of Few‐Layer MoS 2 via In Situ Scanning Transmission Electron Microscopy journal December 2019
Laser Synthesis, Processing, and Spectroscopy of Atomically-Thin Two Dimensional Materials book January 2018
Environmental engineering of transition metal dichalcogenide optoelectronics journal June 2018
Weakened interlayer coupling in two-dimensional MoSe2 flakes with screw dislocations journal June 2019
Recent Progress in the Fabrication, Properties, and Devices of Heterostructures Based on 2D Materials journal February 2019
Van der Waals heterostructures and devices journal July 2016
Layer-by-layer assembly of two-dimensional materials into wafer-scale heterostructures journal September 2017
Supercurrent in van der Waals Josephson junction journal February 2016
Topological mosaics in moiré superlattices of van der Waals heterobilayers journal November 2016
Thickness-modulated metal-to-semiconductor transformation in a transition metal dichalcogenide journal March 2018
2D materials for quantum information science journal August 2019
Helical van der Waals crystals with discretized Eshelby twist journal June 2019
Stacking change in MoS2 bilayers induced by interstitial Mo impurities journal February 2018
Origins of Moiré Patterns in CVD-grown MoS2 Bilayer Structures at the Atomic Scales journal June 2018
Elastic Deformations in 2D van der waals Heterostructures and their Impact on Optoelectronic Properties: Predictions from a Multiscale Computational Approach journal June 2015
Electronic transport properties of transition metal dichalcogenide field-effect devices: surface and interface effects journal January 2015
Spotting the differences in two-dimensional materials – the Raman scattering perspective journal January 2018
Orientation dependent interlayer stacking structure in bilayer MoS 2 domains journal January 2017
Laminated bilayer MoS 2 with weak interlayer coupling journal January 2018
Nanodots of transition metal (Mo and W) disulfides grown on NiNi Prussian blue analogue nanoplates for efficient hydrogen production journal January 2018
The role of Anderson’s rule in determining electronic, optical and transport properties of transition metal dichalcogenide heterostructures journal January 2018
Two-dimensional light-emitting materials: preparation, properties and applications journal January 2018
Photovoltaic effect in a few-layer ReS 2 /WSe 2 heterostructure journal January 2018
Interlayer interactions in 2D WS 2 /MoS 2 heterostructures monolithically grown by in situ physical vapor deposition journal January 2018
Co-adsorption of an anionic dye in the presence of a cationic dye and a heavy metal ion by graphene oxide and photoreduced graphene oxide journal January 2019
Yolk–shell hierarchical catalyst with tremella-like molybdenum sulfide on transition metal (Co, Ni and Fe) sulfide for electrochemical water splitting journal January 2019
Tunable electronic and optical properties of the WS 2 /IGZO heterostructure via an external electric field and strain: a theoretical study journal January 2019
Thermally driven homonuclear-stacking phase of MoS 2 through desulfurization journal January 2019
Direct bilayer growth: a new growth principle for a novel WSe 2 homo-junction and bilayer WSe 2 growth journal January 2020
Construction of van der Waals magnetic tunnel junction using ferromagnetic layered dichalcogenide journal September 2015
First principles study and empirical parametrization of twisted bilayer MoS2 based on band-unfolding journal September 2016
Control of interlayer physics in 2H transition metal dichalcogenides journal December 2017
Suppression of the shear Raman mode in defective bilayer MoS 2 journal February 2019
Band engineering in twisted molybdenum disulfide bilayers journal April 2018
Chemical vapor deposition growth of sub-centimeter single crystal WSe 2 monolayer by NaCl-assistant journal November 2018
Ultralow thermal conductivity of turbostratically disordered MoSe 2 ultra-thin films and implications for heterostructures journal April 2019
Modelling of stacked 2D materials and devices journal August 2015
Systematic study of electronic structure and band alignment of monolayer transition metal dichalcogenides in Van der Waals heterostructures journal November 2016
Vertical heterostructures based on SnSe 2 /MoS 2 for high performance photodetectors journal March 2017
Charge transfer across monolayer/bilayer MoS 2 lateral interface and its influence on exciton and trion characteristics journal January 2019
Mechanical and liquid phase exfoliation of cylindrite: a natural van der Waals superlattice with intrinsic magnetic interactions journal May 2019
Robust circular polarization of indirect Q-K transitions in bilayer 3 R W S 2 journal October 2019
Layer and doping tunable ferromagnetic order in two-dimensional Cr S 2 layers journal June 2018
Moiré excitons: From programmable quantum emitter arrays to spin-orbit–coupled artificial lattices journal November 2017
Valley-polarized exciton dynamics in a 2D semiconductor heterostructure journal February 2016
Dependence of Raman and absorption spectra of stacked bilayer MoS_2 on the stacking orientation journal January 2016
Manufacturing strategies for wafer-scale two-dimensional transition metal dichalcogenide heterolayers journal February 2020
Giant Valley Coherence at Room Temperature in 3R WS 2 with Broken Inversion Symmetry journal October 2019
2D Layered Material-Based van der Waals Heterostructures for Optoelectronics journal January 2018
Controlled Vapor Growth and Nonlinear Optical Applications of Large-Area 3R Phase WS 2 and WSe 2 Atomic Layers journal January 2019
Metallo‐Hydrogel‐Assisted Synthesis and Direct Writing of Transition Metal Dichalcogenides journal May 2019
Controlled Doping of Large-Area Trilayer MoS 2 with Molecular Reductants and Oxidants journal January 2015
Temperature-Mediated Selective Growth of MoS 2 /WS 2 and WS 2 /MoS 2 Vertical Stacks on Au Foils for Direct Photocatalytic Applications journal October 2016
Atomic-Scale Structural Modification of 2D Materials journal January 2019
Stacking-controllable interlayer coupling and symmetric configuration of multilayered MoS2 journal February 2018
Self-organized twist-heterostructures via aligned van der Waals epitaxy and solid-state transformations journal December 2019
Resonantly hybridized excitons in moiré superlattices in van der Waals heterostructures journal March 2019
Tuning the photo-response in monolayer MoS2 by plasmonic nano-antenna journal March 2016
Unveiling exceptionally robust valley contrast in AA- and AB-stacked bilayer WS 2 journal January 2019
Bilayer MoS 2 quantum dots with tunable magnetism and spin journal November 2018
Second harmonic generation in strained transition metal dichalcogenide monolayers: MoS 2 , MoSe 2 , WS 2 , and WSe 2 journal March 2019
Band-edges and band-gap in few-layered transition metal dichalcogenides journal May 2018
Controllable epitaxial growth of MoSe 2 –MoS 2 lateral heterostructures with tunable electrostatic properties journal October 2018
Tailoring excitonic states of van der Waals bilayers through stacking configuration, band alignment, and valley spin journal December 2019
In situ atomic level studies of thermally controlled interlayer stacking shifts in 2D transition metal dichalcogenide bilayers journal January 2020
2D Materials for Optical Modulation: Challenges and Opportunities journal February 2017
Edge-terminated molybdenum disulfide with a 9.4-Å interlayer spacing for electrochemical hydrogen production journal July 2015
Transition metal dichalcogenides bilayer single crystals by reverse-flow chemical vapor epitaxy journal February 2019
Chiral twisted van der Waals nanowires journal April 2019
Raman spectroscopy of transition metal dichalcogenides journal July 2016
Interlayer coupling in two-dimensional semiconductor materials journal August 2018
Inorganic 2D Luminescent Materials: Structure, Luminescence Modulation, and Applications journal October 2019
Anomalous interlayer vibrations in strongly coupled layered PdSe 2 journal May 2018
Optical second harmonic generation in encapsulated single-layer InSe text January 2018
Momentum-space indirect interlayer excitons in transition-metal dichalcogenide van der Waals heterostructures journal April 2018
Optical second harmonic generation in encapsulated single-layer InSe journal October 2018
Anomalous light cones and valley optical selection rules of interlayer excitons in twisted heterobilayers text January 2015
General theoretical description of angle-resolved photoemission spectroscopy of van der Waals structures text January 2017
Momentum-space indirect interlayer excitons in transition metal dichalcogenide van der Waals heterostructures text January 2018
InSe: a two-dimensional material with strong interlayer coupling text January 2018
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