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Title: Origin of band gaps in graphene on hexagonal boron nitride

Abstract

Recent progress in preparing well-controlled two-dimensional van der Waals heterojunctions has opened up a new frontier in materials physics. Here we address the intriguing energy gaps that are sometimes observed when a graphene sheet is placed on a hexagonal boron nitride substrate, demonstrating that they are produced by an interesting interplay between structural and electronic properties, including electronic many-body exchange interactions. Our theory is able to explain the observed gap behaviour by accounting first for the structural relaxation of graphene’s carbon atoms when placed on a boron nitride substrate, and then for the influence of the substrate on low-energy π-electrons located at relaxed carbon atom sites. The methods we employ can be applied to many other van der Waals heterojunctions.

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [4]
  1. National University of Singapore, Department of Physics, Graphene Research Centre, 2 Science Drive 3, Singapore, 117551, Singapore
  2. The University of Texas at Austin, Department of Physics, 2515 Speedway, C1600 Austin, Austin, 78712-1192, Texas (United States)
  3. • The University of Texas at Austin, Department of Physics, 2515 Speedway, C1600 Austin, Austin, 78712-1192, Texas (United States)
  4. Department of Physics, Graphene Research Centre, National University of Singapore, 2 Science Drive 3, Singapore, 117551, Singapore; Yale-NUS College, 6 College Avenue East, Singapore, 138614, Singapore
Publication Date:
Research Org.:
Univ. of Pennsylvania, Philadelphia, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Research Foundation of Singapore; Welch Foundation
OSTI Identifier:
1623965
Grant/Contract Number:  
FG02-84ER45118; NRF-NRFF2012-01; TBF1473
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
Science & Technology - Other Topics

Citation Formats

Jung, Jeil, DaSilva, Ashley M., MacDonald, Allan H., and Adam, Shaffique. Origin of band gaps in graphene on hexagonal boron nitride. United States: N. p., 2015. Web. doi:10.1038/ncomms7308.
Jung, Jeil, DaSilva, Ashley M., MacDonald, Allan H., & Adam, Shaffique. Origin of band gaps in graphene on hexagonal boron nitride. United States. https://doi.org/10.1038/ncomms7308
Jung, Jeil, DaSilva, Ashley M., MacDonald, Allan H., and Adam, Shaffique. Thu . "Origin of band gaps in graphene on hexagonal boron nitride". United States. https://doi.org/10.1038/ncomms7308. https://www.osti.gov/servlets/purl/1623965.
@article{osti_1623965,
title = {Origin of band gaps in graphene on hexagonal boron nitride},
author = {Jung, Jeil and DaSilva, Ashley M. and MacDonald, Allan H. and Adam, Shaffique},
abstractNote = {Recent progress in preparing well-controlled two-dimensional van der Waals heterojunctions has opened up a new frontier in materials physics. Here we address the intriguing energy gaps that are sometimes observed when a graphene sheet is placed on a hexagonal boron nitride substrate, demonstrating that they are produced by an interesting interplay between structural and electronic properties, including electronic many-body exchange interactions. Our theory is able to explain the observed gap behaviour by accounting first for the structural relaxation of graphene’s carbon atoms when placed on a boron nitride substrate, and then for the influence of the substrate on low-energy π-electrons located at relaxed carbon atom sites. The methods we employ can be applied to many other van der Waals heterojunctions.},
doi = {10.1038/ncomms7308},
journal = {Nature Communications},
number = 1,
volume = 6,
place = {United States},
year = {Thu Feb 19 00:00:00 EST 2015},
month = {Thu Feb 19 00:00:00 EST 2015}
}

Works referenced in this record:

Boron nitride substrates for high-quality graphene electronics
journal, August 2010

  • Dean, C. R.; Young, A. F.; Meric, I.
  • Nature Nanotechnology, Vol. 5, Issue 10, p. 722-726
  • DOI: 10.1038/nnano.2010.172

Epitaxial growth of single-domain graphene on hexagonal boron nitride
journal, July 2013

  • Yang, Wei; Chen, Guorui; Shi, Zhiwen
  • Nature Materials, Vol. 12, Issue 9
  • DOI: 10.1038/nmat3695

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

  • Ponomarenko, L. A.; Gorbachev, R. V.; Yu, G. L.
  • Nature, Vol. 497, Issue 7451
  • DOI: 10.1038/nature12187

Hofstadter’s butterfly and the fractal quantum Hall effect in moiré superlattices
journal, May 2013


Field-Effect Tunneling Transistor Based on Vertical Graphene Heterostructures
journal, February 2012


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

  • Yankowitz, Matthew; Xue, Jiamin; Cormode, Daniel
  • Nature Physics, Vol. 8, Issue 5
  • DOI: 10.1038/nphys2272

Substrate-induced band gap in graphene on hexagonal boron nitride: Ab initio density functional calculations
journal, August 2007


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


Graphene on incommensurate substrates: Trigonal warping and emerging Dirac cone replicas with halved group velocity
journal, August 2012


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

  • Woods, C. R.; Britnell, L.; Eckmann, A.
  • Nature Physics, Vol. 10, Issue 6
  • DOI: 10.1038/nphys2954

Mind the gap
journal, October 2007


Generic miniband structure of graphene on a hexagonal substrate
journal, June 2013


Precisely aligned graphene grown on hexagonal boron nitride by catalyst free chemical vapor deposition
journal, September 2013

  • Tang, Shujie; Wang, Haomin; Zhang, Yu
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep02666

Graphene Antidot Lattices: Designed Defects and Spin Qubits
journal, April 2008


Gaps tunable by electrostatic gates in strained graphene
journal, May 2011


Zero-energy modes and gate-tunable gap in graphene on hexagonal boron nitride
journal, September 2012


Pseudospin order in monolayer, bilayer and double-layer graphene
journal, January 2012


Band gaps in incommensurable graphene on hexagonal boron nitride
journal, May 2014


Electron Interactions and Gap Opening in Graphene Superlattices
journal, December 2013


Gapped broken symmetry states in ABC-stacked trilayer graphene
journal, August 2013


Graphene Bilayer with a Twist: Electronic Structure
journal, December 2007

  • Lopes dos Santos, J. M. B.; Peres, N. M. R.; Castro Neto, A. H.
  • Physical Review Letters, Vol. 99, Issue 25
  • DOI: 10.1103/PhysRevLett.99.256802

Quantum Interference at the Twist Boundary in Graphene
journal, August 2008


Localization of Dirac Electrons in Rotated Graphene Bilayers
journal, March 2010

  • Trambly de Laissardière, G.; Mayou, D.; Magaud, L.
  • Nano Letters, Vol. 10, Issue 3
  • DOI: 10.1021/nl902948m

Commensuration and interlayer coherence in twisted bilayer graphene
journal, April 2010


Moire bands in twisted double-layer graphene
journal, July 2011

  • Bistritzer, R.; MacDonald, A. H.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 30
  • DOI: 10.1073/pnas.1108174108

Electronic structure of spontaneously strained graphene on hexagonal boron nitride
journal, September 2014


Approximate modeling of spherical membranes
journal, December 2010


Finite Temperature Lattice Properties of Graphene beyond the Quasiharmonic Approximation
journal, January 2009


Adhesion and electronic structure of graphene on hexagonal boron nitride substrates
journal, November 2011


Gauge field induced by ripples in graphene
journal, May 2008


Gauge fields in graphene
journal, November 2010


Tight-binding model for graphene π -bands from maximally localized Wannier functions
journal, May 2013


Dispersion corrections in graphenic systems: a simple and effective model of binding
journal, October 2013


Effects beyond the random-phase approximation in calculating the interaction between metal films
journal, November 2004


van der Waals Bonding in Layered Compounds from Advanced Density-Functional First-Principles Calculations
journal, June 2012


Gauge field induced by ripples in graphene
text, January 2008


Gauge fields in graphene
text, January 2010


Moire bands in twisted double-layer graphene
text, January 2010


Approximate Modeling of Spherical Membrane
text, January 2010


Gaps tunable by electrostatic gates in strained graphene
text, January 2010


Adhesion and electronic structure of graphene on hexagonal boron nitride substrates
text, January 2011


Cloning of Dirac fermions in graphene superlattices
text, January 2012


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


Epitaxial growth of single-domain graphene on hexagonal boron nitride
journal, July 2013

  • Yang, Wei; Chen, Guorui; Shi, Zhiwen
  • Nature Materials, Vol. 12, Issue 9
  • DOI: 10.1038/nmat3695

Precisely aligned graphene grown on hexagonal boron nitride by catalyst free chemical vapor deposition
journal, September 2013

  • Tang, Shujie; Wang, Haomin; Zhang, Yu
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep02666

Gapped state of a carbon monolayer in periodic magnetic and electric fields
journal, August 2009


Cohesive Properties and Asymptotics of the Dispersion Interaction in Graphite by the Random Phase Approximation
journal, November 2010


First-Principles Description of Correlation Effects in Layered Materials
journal, April 2006


Field-Effect Tunneling Transistor Based on Vertical Graphene Heterostructures
journal, February 2012


Graphene bilayer with a twist: electronic structure
text, January 2007


Graphene Antidot Lattices - Designed Defects and Spin Qubits
text, January 2008


Atomistic simulations of structural and thermodynamic properties of bilayer graphene
text, January 2010


Cloning of Dirac fermions in graphene superlattices
text, January 2012


Works referencing / citing this record:

Van Der Waals Heterostructures with Spin‐Orbit Coupling
journal, December 2019


Boron Nitride Nanostructures: Fabrication, Functionalization and Applications
journal, April 2016


Emerging 0D Transition-Metal Dichalcogenides for Sensors, Biomedicine, and Clean Energy
journal, June 2017


Solitary Waves on Graphene Superlattices
book, December 2017


Temperature Effect on the First Excited State Energy and Average Phonon Number of Bound Magnetopolarons in Monolayer Graphene
journal, May 2019


Band gap opening in graphene: a short theoretical study
journal, March 2017


Pressure-induced commensurate stacking of graphene on boron nitride
journal, October 2016

  • Yankowitz, Matthew; Watanabe, K.; Taniguchi, T.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms13168

Gaps induced by inversion symmetry breaking and second-generation Dirac cones in graphene/hexagonal boron nitride
journal, August 2016

  • Wang, Eryin; Lu, Xiaobo; Ding, Shijie
  • Nature Physics, Vol. 12, Issue 12
  • DOI: 10.1038/nphys3856

Tunable crystal symmetry in graphene–boron nitride heterostructures with coexisting moiré superlattices
journal, September 2019

  • Finney, Nathan R.; Yankowitz, Matthew; Muraleetharan, Lithurshanaa
  • Nature Nanotechnology, Vol. 14, Issue 11
  • DOI: 10.1038/s41565-019-0547-2

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


Dynamic band-structure tuning of graphene moiré superlattices with pressure
journal, May 2018


Conductance signatures of electron confinement induced by strained nanobubbles in graphene
journal, January 2015

  • Bahamon, Dario A.; Qi, Zenan; Park, Harold S.
  • Nanoscale, Vol. 7, Issue 37
  • DOI: 10.1039/c5nr03393d

Superlattices based on van der Waals 2D materials
journal, January 2019

  • Ryu, Yu Kyoung; Frisenda, Riccardo; Castellanos-Gomez, Andres
  • Chemical Communications, Vol. 55, Issue 77
  • DOI: 10.1039/c9cc04919c

Charge transport and electron-hole asymmetry in low-mobility graphene/hexagonal boron nitride heterostructures
journal, February 2018

  • Li, Jiayu; Lin, Li; Huang, Guang-Yao
  • Journal of Applied Physics, Vol. 123, Issue 6
  • DOI: 10.1063/1.5009742

Substitutional mechanism for growth of hexagonal boron nitride on epitaxial graphene
journal, July 2018

  • Mende, Patrick C.; Li, Jun; Feenstra, Randall M.
  • Applied Physics Letters, Vol. 113, Issue 3
  • DOI: 10.1063/1.5039823

Electronic transport and Klein tunneling in gapped AA-stacked bilayer graphene
journal, November 2018

  • Abdullah, Hasan M.; Al Ezzi, Mohammed; Bahlouli, H.
  • Journal of Applied Physics, Vol. 124, Issue 20
  • DOI: 10.1063/1.5052402

Microwave second-harmonic generation due to mobile carriers in doped graphene lacking center-of-inversion symmetry
journal, August 2019

  • Margulis, Vl. A.; Muryumin, E. E.
  • Journal of Applied Physics, Vol. 126, Issue 5
  • DOI: 10.1063/1.5111506

Topological phases in two-dimensional materials: a review
journal, May 2016


Electronic and optical properties of strained graphene and other strained 2D materials: a review
journal, August 2017

  • Naumis, Gerardo G.; Barraza-Lopez, Salvador; Oliva-Leyva, Maurice
  • Reports on Progress in Physics, Vol. 80, Issue 9
  • DOI: 10.1088/1361-6633/aa74ef

Interband scattering-induced ambipolar transport in graphene
journal, May 2019

  • Iglesias, José Manuel; Pascual, Elena; Hamham, El Mokhtar
  • Semiconductor Science and Technology, Vol. 34, Issue 6
  • DOI: 10.1088/1361-6641/ab2087

Valley Hall transport of photon-dressed quasiparticles in two-dimensional Dirac semiconductors
journal, August 2018


Structural and electronic transformation in low-angle twisted bilayer graphene
journal, November 2017


Quasiparticle electronic structure of honeycomb C 3 N: from monolayer to bulk
journal, November 2018


Pressure induced compression of flatbands in twisted bilayer graphene
journal, November 2018

  • Chittari, Bheema Lingam; Leconte, Nicolas; Javvaji, Srivani
  • Electronic Structure, Vol. 1, Issue 1
  • DOI: 10.1088/2516-1075/aaead3

Polaritonic contribution to the Casimir energy between two graphene layers
journal, December 2019


Determining graphene's induced band gap with magnetic and electric emitters
journal, February 2016


Interlayer transport through a graphene/rotated boron nitride/graphene heterostructure
journal, January 2017


Stacking in incommensurate graphene/hexagonal-boron-nitride heterostructures based on ab initio study of interlayer interaction
journal, August 2017


Crystal-field effects in graphene with interface-induced spin-orbit coupling
journal, July 2018


Substrate-induced topological minibands in graphene
journal, September 2018


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


Evidence for a fractional fractal quantum Hall effect in graphene superlattices
journal, December 2015


Emergent ferromagnetism near three-quarters filling in twisted bilayer graphene
journal, July 2019


Conductance signatures of electron confinement induced by strained nanobubbles in graphene
text, January 2015


Topological Phases in Two-Dimensional Materials: A Brief Review
text, January 2015


Determining graphene's induced band gap with magnetic and electric emitters
text, January 2016


Pressure-induced commensurate stacking of graphene on boron nitride
text, January 2016


Electronic Structure Theory of Weakly Interacting Bilayers
text, January 2016


Structural and electronic transformation in low-angle twisted bilayer graphene
text, January 2017


Electronic spectrum of twisted graphene layers under heterostrain
text, January 2018


Substrate-induced topological minibands in graphene
text, January 2018


Pressure-Induced Metal-Insulator Transition in Twisted Bi-layer Graphene
text, January 2018


Van der Waals heterostructures with spin-orbit coupling
text, January 2019


Polaritonic Contribution to the Casimir Energy between two Graphene Layers
text, January 2019


Chirality-Induced Giant Unidirectional Magnetoresistance in Twisted Bilayer Graphene
journal, February 2021


Quantifying electronic band interactions in van der Waals materials using angle-resolved reflected-electron spectroscopy
journal, November 2016

  • Jobst, Johannes; van der Torren, Alexander J. H.; Krasovskii, Eugene E.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms13621

Spin-triplet superconductivity from intervalley Goldstone modes in magic-angle graphene
journal, December 2022


Novel effects of strains in graphene and other two dimensional materials
text, January 2015


THz conductivity of graphene on boron nitride
text, January 2015


Pressure-induced commensurate stacking of graphene on boron nitride
text, January 2016


Giant modulation of the electronic band gap of carbon nanotubes by dielectric screening
text, January 2016


Periodically Gated Bilayer Graphene as an Electronic Metamaterial
text, January 2020