skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Structural, electronic, vibrational, and elastic properties of graphene/ MoS 2 bilayer heterostructures

Abstract

Graphene/MoS2 van der Waals (vdW) heterostructures have promising technological applications due to their unique properties and functionalities. Many experimental and theoretical research groups across the globe have made outstanding contributions to benchmark the properties of graphene/MoS2 heterostructures. Even though some research groups have modeled the graphene/MoS2 heterostructures using first-principles calculations, there exist several discrepancies in the results from different theoretical research groups and the experimental findings. In the present work, we revisit this problem by means of first-principles calculations and address the existing discrepancies about the interlayer spacing between graphene and MoS2 monolayers in graphene/MoS2 heterostructures and about the location of Dirac points near the Fermi level. We further investigate the electronic, mechanical, and vibrational properties of the optimized graphene/MoS2 heterostructures created using 5 x 5/4 x 4 and 4 x 4/3 x 3 supercell geometries having different magnitudes of lattice mismatch. The effect of the varying interlayer spacing on the electronic properties of heterostructures is discussed. Our phonon calculations reveal that the interlayer shear and breathing phonon modes, which are very sensitive to the weak vdW interactions, play a vital role in describing the thermal properties of the studied systems. The thermodynamic and elastic properties of heterostructures are furthermore » discussed. A systematic comparison between our results and the results reported from other research groups is presented.« less

Authors:
; ;
Publication Date:
Research Org.:
West Virginia Univ., Morgantown, WV (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Contributing Org.:
This work used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation Grant No. OCI-1053575. Additionally, the authors acknowledge the support from Texas Advances Computer Center (TACC), Bridges supercomputer at Pittsburgh Supercomputer Center and Super Computing Systems (Spruce and Mountaineer) at West Virginia University (WVU). A.H.R. and S.S. acknowledge the support from National Science Foundation (NSF) DMREF-NSF 1434897and DOE DE-SC0016176 projects. S.S. thanks the donors of the Jefimenko family for their financial support through the Oleg D. and Valentina P. Jefimenko Physics Fellowship at WVU. S.S. also acknowledges the support from the Robert T. Bruhn research award, the WVU Foundation Distinguished Doctoral Fellowship, and Dr. Mohindar S. Seehra Research Award. C.E. acknowledges support from Dirección de Investigación, Creación y Extensión at UTADEO. We thank Prof. Sergio E. Ulloa for fruitful discussions.
OSTI Identifier:
1593982
Alternate Identifier(s):
OSTI ID: 1477563
Grant/Contract Number:  
SC0016176
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 98; Journal Issue: 15; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Singh, Sobhit, Espejo, Camilo, and Romero, Aldo H. Structural, electronic, vibrational, and elastic properties of graphene/ MoS2 bilayer heterostructures. United States: N. p., 2018. Web. doi:10.1103/PhysRevB.98.155309.
Singh, Sobhit, Espejo, Camilo, & Romero, Aldo H. Structural, electronic, vibrational, and elastic properties of graphene/ MoS2 bilayer heterostructures. United States. doi:10.1103/PhysRevB.98.155309.
Singh, Sobhit, Espejo, Camilo, and Romero, Aldo H. Mon . "Structural, electronic, vibrational, and elastic properties of graphene/ MoS2 bilayer heterostructures". United States. doi:10.1103/PhysRevB.98.155309. https://www.osti.gov/servlets/purl/1593982.
@article{osti_1593982,
title = {Structural, electronic, vibrational, and elastic properties of graphene/ MoS2 bilayer heterostructures},
author = {Singh, Sobhit and Espejo, Camilo and Romero, Aldo H.},
abstractNote = {Graphene/MoS2 van der Waals (vdW) heterostructures have promising technological applications due to their unique properties and functionalities. Many experimental and theoretical research groups across the globe have made outstanding contributions to benchmark the properties of graphene/MoS2 heterostructures. Even though some research groups have modeled the graphene/MoS2 heterostructures using first-principles calculations, there exist several discrepancies in the results from different theoretical research groups and the experimental findings. In the present work, we revisit this problem by means of first-principles calculations and address the existing discrepancies about the interlayer spacing between graphene and MoS2 monolayers in graphene/MoS2 heterostructures and about the location of Dirac points near the Fermi level. We further investigate the electronic, mechanical, and vibrational properties of the optimized graphene/MoS2 heterostructures created using 5 x 5/4 x 4 and 4 x 4/3 x 3 supercell geometries having different magnitudes of lattice mismatch. The effect of the varying interlayer spacing on the electronic properties of heterostructures is discussed. Our phonon calculations reveal that the interlayer shear and breathing phonon modes, which are very sensitive to the weak vdW interactions, play a vital role in describing the thermal properties of the studied systems. The thermodynamic and elastic properties of heterostructures are further discussed. A systematic comparison between our results and the results reported from other research groups is presented.},
doi = {10.1103/PhysRevB.98.155309},
journal = {Physical Review B},
number = 15,
volume = 98,
place = {United States},
year = {2018},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 5 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Phonon dispersions and vibrational properties of monolayer, bilayer, and trilayer graphene: Density-functional perturbation theory
journal, March 2008


Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Graphene spintronics
journal, October 2014

  • Han, Wei; Kawakami, Roland K.; Gmitra, Martin
  • Nature Nanotechnology, Vol. 9, Issue 10
  • DOI: 10.1038/nnano.2014.214

MoS 2 : Choice Substrate for Accessing and Tuning the Electronic Properties of Graphene
journal, October 2014


Nonlinear elastic behavior of two-dimensional molybdenum disulfide
journal, January 2013


Band-structure topologies of graphene: Spin-orbit coupling effects from first principles
journal, December 2009


Interlayer screening effect in graphene multilayers with A B A and A B C stacking
journal, March 2010


Band Alignment and Minigaps in Monolayer MoS 2 -Graphene van der Waals Heterostructures
journal, June 2016


Mechanical properties of graphene and boronitrene
journal, March 2012


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

  • Deng, Dehui; Novoselov, K. S.; Fu, Qiang
  • Nature Nanotechnology, Vol. 11, Issue 3
  • DOI: 10.1038/nnano.2015.340

Emerging Photoluminescence in Monolayer MoS2
journal, April 2010

  • Splendiani, Andrea; Sun, Liang; Zhang, Yuanbo
  • Nano Letters, Vol. 10, Issue 4, p. 1271-1275
  • DOI: 10.1021/nl903868w

Nonvolatile Memory Cells Based on MoS 2 /Graphene Heterostructures
journal, March 2013

  • Bertolazzi, Simone; Krasnozhon, Daria; Kis, Andras
  • ACS Nano, Vol. 7, Issue 4
  • DOI: 10.1021/nn3059136

Graphene–MoS2 hybrid structures for multifunctional photoresponsive memory devices
journal, October 2013

  • Roy, Kallol; Padmanabhan, Medini; Goswami, Srijit
  • Nature Nanotechnology, Vol. 8, Issue 11
  • DOI: 10.1038/nnano.2013.206

Lithium Intercalation in Graphene/MoS 2 Composites: First-Principles Insights
journal, November 2015

  • Shao, Xiji; Wang, Kedong; Pang, Rui
  • The Journal of Physical Chemistry C, Vol. 119, Issue 46
  • DOI: 10.1021/acs.jpcc.5b06441

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Proximity Effects in Bilayer Graphene on Monolayer WSe 2 : Field-Effect Spin Valley Locking, Spin-Orbit Valve, and Spin Transistor
journal, October 2017


Band structure tunability in MoS 2 under interlayer compression: A DFT and GW study
journal, June 2013


Recent developments in the ABINIT software package
journal, August 2016


Band Offset and Negative Compressibility in Graphene-MoS 2 Heterostructures
journal, March 2014

  • Larentis, Stefano; Tolsma, John R.; Fallahazad, Babak
  • Nano Letters, Vol. 14, Issue 4
  • DOI: 10.1021/nl500212s

Van der Waals Epitaxy of Two-Dimensional MoS 2 –Graphene Heterostructures in Ultrahigh Vacuum
journal, May 2015


Accurate Molecular Van Der Waals Interactions from Ground-State Electron Density and Free-Atom Reference Data
journal, February 2009


Optimized norm-conserving Vanderbilt pseudopotentials
journal, August 2013


Graphane: A two-dimensional hydrocarbon
journal, April 2007


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


Controlling the magnetic and optical responses of a MoS 2 monolayer by lanthanide substitutional doping: a first-principles study
journal, January 2017

  • Ouma, Cecil N. M.; Singh, Sobhit; Obodo, Kingsley O.
  • Physical Chemistry Chemical Physics, Vol. 19, Issue 37
  • DOI: 10.1039/C7CP03160B

Bilayer graphene under pressure: Electron-hole symmetry breaking, valley Hall effect, and Landau levels
journal, June 2016


Outstanding mechanical properties of monolayer MoS2 and its application in elastic energy storage
journal, January 2013

  • Peng, Qing; De, Suvranu
  • Physical Chemistry Chemical Physics, Vol. 15, Issue 44
  • DOI: 10.1039/c3cp52879k

The electronic properties of graphene
journal, January 2009

  • Castro Neto, A. H.; Guinea, F.; Peres, N. M. R.
  • Reviews of Modern Physics, Vol. 81, Issue 1, p. 109-162
  • DOI: 10.1103/RevModPhys.81.109

First-principles investigation of MoS 2 monolayer adsorbed on SiO 2 (0001) Surface
journal, September 2017


Modelling of stacked 2D materials and devices
journal, August 2015


Large excitonic effects in monolayers of molybdenum and tungsten dichalcogenides
journal, September 2012


In situ catalytic growth of large-area multilayered graphene/MoS2 heterostructures
journal, April 2014

  • Fu, Wei; Du, Fei-Hu; Su, Juan
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep04673

Controlled charge trapping by molybdenum disulphide and graphene in ultrathin heterostructured memory devices
journal, March 2013

  • Sup Choi, Min; Lee, Gwan-Hyoung; Yu, Young-Jun
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2652

Mass inversion in graphene by proximity to dichalcogenide monolayer
journal, December 2016

  • Alsharari, Abdulrhman M.; Asmar, Mahmoud M.; Ulloa, Sergio E.
  • Physical Review B, Vol. 94, Issue 24
  • DOI: 10.1103/PhysRevB.94.241106

Trivial and inverted Dirac bands and the emergence of quantum spin Hall states in graphene on transition-metal dichalcogenides
journal, April 2016


Asymmetry gap in the electronic band structure of bilayer graphene
journal, October 2006


Measurement of the Elastic Properties and Intrinsic Strength of Monolayer Graphene
journal, July 2008


A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010

  • Grimme, Stefan; Antony, Jens; Ehrlich, Stephan
  • The Journal of Chemical Physics, Vol. 132, Issue 15
  • DOI: 10.1063/1.3382344

Effects of interlayer coupling and electric fields on the electronic structures of graphene and MoS 2 heterobilayers
journal, January 2016

  • Hu, Wei; Wang, Tian; Zhang, Ruiqi
  • Journal of Materials Chemistry C, Vol. 4, Issue 9
  • DOI: 10.1039/C6TC00207B

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965


Graphene on transition-metal dichalcogenides: A platform for proximity spin-orbit physics and optospintronics
journal, October 2015


Effect of the damping function in dispersion corrected density functional theory
journal, March 2011

  • Grimme, Stefan; Ehrlich, Stephan; Goerigk, Lars
  • Journal of Computational Chemistry, Vol. 32, Issue 7
  • DOI: 10.1002/jcc.21759

Ultrahigh-Gain Photodetectors Based on Atomically Thin Graphene-MoS2 Heterostructures
journal, January 2014

  • Zhang, Wenjing; Chuu, Chih-Piao; Huang, Jing-Kai
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep03826

Vibrational properties of graphene and graphene layers
journal, December 2009

  • Wang, Hui; Wang, Yufang; Cao, Xuewei
  • Journal of Raman Spectroscopy, Vol. 40, Issue 12
  • DOI: 10.1002/jrs.2321

The PseudoDojo: Training and grading a 85 element optimized norm-conserving pseudopotential table
journal, May 2018


Investigation of novel crystal structures of Bi–Sb binaries predicted using the minima hopping method
journal, January 2016

  • Singh, Sobhit; Ibarra-Hernández, Wilfredo; Valencia-Jaime, Irais
  • Physical Chemistry Chemical Physics, Vol. 18, Issue 43
  • DOI: 10.1039/C6CP05401C

Tunable MoS 2 bandgap in MoS 2 -graphene heterostructures
journal, July 2014

  • Ebnonnasir, Abbas; Narayanan, Badri; Kodambaka, Suneel
  • Applied Physics Letters, Vol. 105, Issue 3
  • DOI: 10.1063/1.4891430

Biased Bilayer Graphene: Semiconductor with a Gap Tunable by the Electric Field Effect
journal, November 2007


Origin of layer dependence in band structures of two-dimensional materials
journal, April 2017


Giant tunable Rashba spin splitting in a two-dimensional BiSb monolayer and in BiSb/AlN heterostructures
journal, April 2017


Design of Mg alloys: The effects of Li concentration on the structure and elastic properties in the Mg-Li binary system by first principles calculations
journal, January 2017


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


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

  • Zhao, Yanyuan; Luo, Xin; Li, Hai
  • Nano Letters, Vol. 13, Issue 3
  • DOI: 10.1021/nl304169w

Debye temperature and stiffness of carbon and boron nitride polymorphs from first principles calculations
journal, February 2006


Heterostructures of transition metal dichalcogenides
journal, August 2015


Elastic, mechanical, and thermodynamic properties of Bi-Sb binaries: Effect of spin-orbit coupling
journal, February 2018


Interatomic force constants including the DFT-D dispersion contribution
journal, April 2016


Structural and Electronic Properties of Superlattice Composed of Graphene and Monolayer MoS 2
journal, July 2013

  • Li, X. D.; Yu, S.; Wu, S. Q.
  • The Journal of Physical Chemistry C, Vol. 117, Issue 29
  • DOI: 10.1021/jp404080z

Prediction and control of spin polarization in a Weyl semimetallic phase of BiSb
journal, October 2016


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


Electric Field Effect in Atomically Thin Carbon Films
journal, October 2004


A review on the flexural mode of graphene: lattice dynamics, thermal conduction, thermal expansion, elasticity and nanomechanical resonance
journal, January 2015


First-principles study of the phonon vibrational spectra and thermal properties of hexagonal MoS2
journal, February 2015


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Gate-Voltage Control of Oxygen Diffusion on Graphene
journal, April 2011


Tight-binding theory of the spin-orbit coupling in graphene
journal, December 2010


Graphene versus MoS2: A short review
journal, February 2015


Inhomogeneous Electron Gas
journal, November 1964


Elastic Properties of Chemical-Vapor-Deposited Monolayer MoS 2 , WS 2 , and Their Bilayer Heterostructures
journal, August 2014

  • Liu, Kai; Yan, Qimin; Chen, Michelle
  • Nano Letters, Vol. 14, Issue 9
  • DOI: 10.1021/nl501793a

The phonon dispersion of graphite revisited
journal, July 2004


Semiempirical GGA-type density functional constructed with a long-range dispersion correction
journal, January 2006

  • Grimme, Stefan
  • Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799
  • DOI: 10.1002/jcc.20495

A roadmap for graphene
journal, October 2012

  • Novoselov, K. S.; Fal′ko, V. I.; Colombo, L.
  • Nature, Vol. 490, Issue 7419
  • DOI: 10.1038/nature11458

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


The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets
journal, April 2013

  • Chhowalla, Manish; Shin, Hyeon Suk; Eda, Goki
  • Nature Chemistry, Vol. 5, Issue 4, p. 263-275
  • DOI: 10.1038/nchem.1589

Rotationally Commensurate Growth of MoS 2 on Epitaxial Graphene
journal, November 2015


Nonlinear elastic behavior of graphene: Ab initio calculations to continuum description
journal, November 2009


First-principles calculations of the ferroelastic transition between rutile-type and CaCl 2 -type SiO 2 at high pressures
journal, October 2008


Interface strain in vertically stacked two-dimensional heterostructured carbon-MoS2 nanosheets controls electrochemical reactivity
journal, June 2016

  • Oakes, Landon; Carter, Rachel; Hanken, Trevor
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms11796

Graphene/MoS 2 Hybrid Technology for Large-Scale Two-Dimensional Electronics
journal, May 2014

  • Yu, Lili; Lee, Yi-Hsien; Ling, Xi
  • Nano Letters, Vol. 14, Issue 6
  • DOI: 10.1021/nl404795z

Graphene/ MoS 2 heterostructures as templates for growing two-dimensional metals: Predictions from ab initio calculations
journal, September 2017


Interlayer Interactions in van der Waals Heterostructures: Electron and Phonon Properties
journal, February 2016

  • Le, Nam B.; Huan, Tran Doan; Woods, Lilia M.
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 9
  • DOI: 10.1021/acsami.6b00285

Single-layer MoS2 transistors
journal, January 2011

  • Radisavljevic, B.; Radenovic, A.; Brivio, J.
  • Nature Nanotechnology, Vol. 6, Issue 3, p. 147-150
  • DOI: 10.1038/nnano.2010.279

Pressure-Induced Charge Transfer Doping of Monolayer Graphene/MoS 2 Heterostructure
journal, June 2016


Electric Field and Strain Effect on Graphene-MoS 2 Hybrid Structure: Ab Initio Calculations
journal, July 2015


Observation of an Electric-Field-Induced Band Gap in Bilayer Graphene by Infrared Spectroscopy
journal, June 2009


Graphene adhesion on MoS2 monolayer: An ab initio study
journal, January 2011


The Phenomena of Rupture and Flow in Solids
journal, January 1921

  • Griffith, A. A.
  • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 221, Issue 582-593
  • DOI: 10.1098/rsta.1921.0006