Disorder in van der waals heterostructures of 2d materials

ABSTRACT Realizing the full potential of any materials system requires understanding and controlling disorder, which can obscure intrinsic properties and hinder device performance. Here we

examine both intrinsic and extrinsic disorder in two-dimensional (2D) materials, in particular graphene and transition metal dichalcogenides (TMDs). Minimizing disorder is crucial for

realizing desired properties in 2D materials and improving device performance and repeatability for practical applications. We discuss the progress in disorder control for graphene and TMDs,

as well as in van der Waals heterostructures realized by combining these materials with hexagonal boron nitride. Furthermore, we showcase how atomic defects or disorder can also be

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subscriptions * Read our FAQs * Contact customer support SIMILAR CONTENT BEING VIEWED BY OTHERS BANDGAP ENGINEERING OF TWO-DIMENSIONAL SEMICONDUCTOR MATERIALS Article Open access 24 August

2020 STRAIN ENGINEERING OF 2D SEMICONDUCTORS AND GRAPHENE: FROM STRAIN FIELDS TO BAND-STRUCTURE TUNING AND PHOTONIC APPLICATIONS Article Open access 23 November 2020 UNDERSTANDING EPITAXIAL

GROWTH OF TWO-DIMENSIONAL MATERIALS AND THEIR HOMOSTRUCTURES Article 10 July 2024 REFERENCES * Ma, N. & Jena, D. Charge scattering and mobility in atomically thin semiconductors. _Phys.

Rev. X_ 4, 011043 (2014). Google Scholar  * Sachs, B., Wehling, T. O., Katsnelson, M. I. & Lichtenstein, A. I. Midgap states and band gap modification in defective graphene/h-BN

heterostructures. _Phys. Rev. B_ 94, 224105 (2016). Google Scholar  * Wang, H., Zhang, C. & Rana, F. Ultrafast dynamics of defect-assisted electron hole recombination in monolayer MoS2.

_Nano Lett._ 15, 339–345 (2015). CAS  Google Scholar  * Tsen, A. W. et al. Tailoring electrical transport across grain boundaries in polycrystalline graphene. _Science_ 336, 1143–1146

(2012). CAS  Google Scholar  * Wang, D. et al. Bandgap broadening at grain boundaries in single-layer MoS2. _Nano Res._ 11, 6102–6109 (2018). CAS  Google Scholar  * Hus, S. M. & Li,

A.-P. Spatially-resolved studies on the role of defects and boundaries in electronic behavior of 2D materials. _Prog. Surf. Sci._ 92, 176–201 (2017). CAS  Google Scholar  * Huang, P. Y. et

al. Grains and grain boundaries in single-layer graphene atomic patchwork quilts. _Nature_ 469, 389–392 (2011). CAS  Google Scholar  * Novoselov, K. S. et al. Two-dimensional gas of massless

Dirac fermions in graphene. _Nature_ 438, 197–200 (2005). CAS  Google Scholar  * Martin, J. et al. Observation of electron-hole puddles in graphene using a scanning single-electron

transistor. _Nat. Phys._ 4, 144–148 (2008). CAS  Google Scholar  * Xue, J. et al. Scanning tunnelling microscopy and spectroscopy of ultra-flat graphene on hexagonal boron nitride. _Nat.

Mater._ 10, 282–285 (2011). CAS  Google Scholar  * Decker, R. et al. Local electronic properties of graphene on a BN substrate via scanning tunneling microscopy. _Nano Lett._ 11, 2291–2295

(2011). CAS  Google Scholar  * Zhang, Y., Brar, V. W., Girit, C., Zettl, A. & Crommie, M. F. Origin of spatial charge inhomogeneity in graphene. _Nat. Phys._ 5, 722–726 (2009). CAS 

Google Scholar  * Chen, J.-H. et al. Charged-impurity scattering in graphene. _Nat. Phys._ 4, 377–381 (2008). CAS  Google Scholar  * Adam, S., Hwang, E. H., Galitski, V. M. & Sarma, S.

D. A self-consistent theory for graphene transport. _Proc. Natl Acad. Sci. USA_ 104, 18392–18397 (2007). CAS  Google Scholar  * Shin, B. G. et al. Indirect bandgap puddles in monolayer MoS2

by substrate-induced local strain. _Adv. Mater._ 28, 9378–9384 (2016). CAS  Google Scholar  * Du, X., Skachko, I., Barker, A. & Andrei, E. Y. Approaching ballistic transport in suspended

graphene. _Nat. Nanotechnol._ 3, 491–495 (2008). CAS  Google Scholar  * Bolotin, K. I., Ghahari, F., Shulman, M. D., Stormer, H. L. & Kim, P. Observation of the fractional quantum Hall

effect in graphene. _Nature_ 462, 196–199 (2009). CAS  Google Scholar  * Feldman, B. E., Krauss, B., Smet, J. H. & Yacoby, A. Unconventional sequence of fractional quantum hall states in

suspended graphene. _Science_ 337, 1196–1199 (2012). CAS  Google Scholar  * Jr, J. V. et al. Transport spectroscopy of symmetry-broken insulating states in bilayer graphene. _Nat.

Nanotechnol._ 7, 156–160 (2012). Google Scholar  * Nam, Y., Ki, D.-K., Soler-Delgado, D. & Morpurgo, A. F. Electronhole collision limited transport in charge-neutral bilayer graphene.

_Nat. Phys._ 13, 1207–1214 (2017). CAS  Google Scholar  * Geim, A. K. & Grigorieva, I. V. Van der Waals heterostructures. _Nature_ 499, 419–425 (2013). CAS  Google Scholar  * Favron, A.

et al. Photooxidation and quantum confinement effects in exfoliated black phosphorus. _Nat. Mater._ 14, 826–832 (2015). CAS  Google Scholar  * Taniguchi, T. & Watanabe, K. Synthesis of

high-purity boron nitride single crystals under high pressure by using BaBN solvent. _J. Cryst. Growth_ 303, 525–529 (2007). CAS  Google Scholar  * Dean, C. R. et al. Boron nitride

substrates for high-quality graphene electronics. _Nat. Nanotechnol._ 5, 722–726 (2010). CAS  Google Scholar  * Garcia, A. G. F. et al. Effective cleaning of hexagonal boron nitride for

graphene devices. _Nano Lett._ 12, 4449–4454 (2012). CAS  Google Scholar  * Ponomarenko, L. A. et al. Tunable metalinsulator transition in double-layer graphene heterostructures. _Nat.

Phys._ 7, 958–961 (2011). CAS  Google Scholar  * Wang, L. et al. One-dimensional electrical contact to a two-dimensional material. _Science_ 342, 614–617 (2013). CAS  Google Scholar  *

Osvald, J. On barrier height inhomogeneities at polycrystalline metal-semiconductor contacts. _Solid-State Electron._ 35, 1629–1632 (1992). CAS  Google Scholar  * Zibrov, A. A. et al.

Tunable interacting composite fermion phases in a half-filled bilayer-graphene Landau level. _Nature_ 549, 360–364 (2017). CAS  Google Scholar  * Adam, S. & Das Sarma, S. Transport in

suspended graphene. _Solid State Commun._ 146, 356–360 (2008). CAS  Google Scholar  * Du, X., Skachko, I., Duerr, F., Luican, A. & Andrei, E. Y. Fractional quantum Hall effect and

insulating phase of Dirac electrons in graphene. _Nature_ 462, 192–195 (2009). CAS  Google Scholar  * Banszerus, L. et al. Ballistic transport exceeding 28 µm in CVD grown graphene. _Nano

Lett._ 16, 1387–1391 (2016). CAS  Google Scholar  * Wang, L. et al. Evidence for a fractional fractal quantum Hall effect in graphene superlattices. _Science_ 350, 1231–1234 (2015). CAS 

Google Scholar  * Chen, S. et al. Competing fractional quantum hall and electron solid phases in graphene. _Phys. Rev. Lett._ 122, 026802 (2019). CAS  Google Scholar  * Zibrov, A. A. et al.

Even-denominator fractional quantum hall states at an isospin transition in monolayer graphene. _Nat. Phys._ 14, 930–935 (2018). CAS  Google Scholar  * Zeng, Y. et al. Ultra-high quality

magnetotransport in graphene using the edge-free Corbino geometry. _Phys. Rev. Lett._ 122, 137701 (2019). CAS  Google Scholar  * Schreiber, K. A. et al. Onset of quantum criticality in the

topological-to-nematic transition in a two-dimensional electron gas at filling factor _ν_ = 5_/_2. _Phys. Rev. B_ 96, 041107 (2017). Google Scholar  * Shi, Q. et al. Microwave

photoresistance in an ultra-high-quality GaAs quantum well. _Phys. Rev. B_ 93, 121305 (2016). Google Scholar  * Pan, W., Baldwin, K. W., West, K. W., Pfeiffer, L. N. & Tsui, D. C.

Fractional quantum Hall effect at Landau level filling _ν_ = 4_/_11. _Phys. Rev. B_ 91, 041301 (2015). Google Scholar  * Koulakov, A. A., Fogler, M. M. & Shklovskii, B. I. Charge density

wave in two-dimensional electron liquid in weak magnetic field. _Phys. Rev. Lett._ 76, 499–502 (1996). CAS  Google Scholar  * Forsythe, C. et al. Band structure engineering of 2d materials

using patterned dielectric superlattices. _Nat. Nanotechnol._ 13, 566–571 (2018). CAS  Google Scholar  * Li, J. et al. Negative coulomb drag in double bilayer graphene. _Phys. Rev. Lett._

117, 046802 (2016). CAS  Google Scholar  * Dean, C. R. et al. Hofstadters butterfly and the fractal quantum Hall effect in moiré superlattices. _Nature_ 497, 598–602 (2013). CAS  Google

Scholar  * Yu, G. L. et al. Hierarchy of Hofstadter states and replica quantum Hall ferromagnetism in graphene superlattices. _Nat. Phys._ 10, 525–529 (2014). CAS  Google Scholar  * Cao, Y.

et al. Unconventional superconductivity in magic-angle graphene superlattices. _Nature_ 556, 43–50 (2018). CAS  Google Scholar  * Wang, Q. H., Kalantar-Zadeh, K., Kis, A., Coleman, J. N.

& Strano, M. S. Electronics and optoelectronics of two-dimensional transition metal dichalcogenides. _Nat. Nanotechnol._ 7, 699–712 (2012). CAS  Google Scholar  * Yu, Z. et al.

Realization of room-temperature phonon-limited carrier transport in monolayer MoS2 by dielectric and carrier screening. _Adv. Mater._ 28, 547–552 (2016). CAS  Google Scholar  * Cui, X. et

al. Multi-terminal transport measurements of MoS2 using a van der Waals heterostructure device platform. _Nat. Nanotechnol._ 10, 534–540 (2015). CAS  Google Scholar  * Pisoni, R. et al.

Interactions and magnetotransport through spin-valley coupled Landau levels in monolayer MoS2. _Phys. Rev. Lett._ 121, 247701 (2018). CAS  Google Scholar  * Baugher, B. W. H., Churchill, H.

O. H., Yang, Y. & Jarillo-Herrero, P. Intrinsic electronic transport properties of high-quality monolayer and bilayer MoS2. _Nano Lett._ 13, 4212–4216 (2013). CAS  Google Scholar  *

Radisavljevic, B. & Kis, A. Mobility engineering and a metalinsulator transition in monolayer MoS2. _Nat. Mater._ 12, 815–820 (2013). CAS  Google Scholar  * Late, D. J., Liu, B., Matte,

H. S. S. R., Dravid, V. P. & Rao, C. N. R. Hysteresis in single-layer MoS2 field effect transistors. _ACS Nano_ 6, 5635–5641 (2012). CAS  Google Scholar  * Fallahazad, B. et al.

Shubnikov–de Haas oscillations of high-mobility holes in monolayer and bilayer WSe2: Landau level degeneracy, effective mass, and negative compressibility. _Phys. Rev. Lett._ 116, 086601

(2016). Google Scholar  * Staley, N. E. et al. Electric field effect on superconductivity in atomically thin flakes of NbSe2. _Phys. Rev. B_ 80, 184505 (2009). Google Scholar  * Xi, X. et

al. Ising pairing in superconducting NbSe2 atomic layers. _Nat. Phys._ 12, 139–143 (2016). CAS  Google Scholar  * Huang, B. et al. Layer-dependent ferromagnetism in a van der Waals crystal

down to the monolayer limit. _Nature_ 546, 270–273 (2017). CAS  Google Scholar  * Li, L. et al. Quantum Hall effect in black phosphorus two-dimensional electron system. _Nat. Nanotechnol._

11, 593–597 (2016). CAS  Google Scholar  * Cadiz, F. et al. Excitonic linewidth approaching the homogeneous limit in MoS2-based van der Waals heterostructures. _Phys. Rev. X_ 7, 021026

(2017). Google Scholar  * Ajayi, O. A. et al. Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers. _2D Mater._ 4, 031011 (2017). Google

Scholar  * Zhang, X.-X. et al. Magnetic brightening and control of dark excitons in monolayer WSe2. _Nat. Nanotechnol._ 12, 883–888 (2017). CAS  Google Scholar  * Movva, H. C. et al.

Density-dependent quantum hall states and zeeman splitting in monolayer and bilayer WSe2. _Phys. Rev. Lett._ 118, 247701 (2017). Google Scholar  * Wang, Z., Shan, J. & Mak, K. F. Valley-

and spin-polarized Landau levels in monolayer WSe2. _Nat. Nanotechnol._ 12, 144–149 (2017). CAS  Google Scholar  * You, Y. et al. Observation of biexcitons in monolayer WSe2. _Nat. Phys._

11, 477–481 (2015). CAS  Google Scholar  * Zhou, W. et al. Intrinsic structural defects in monolayer molybdenum disulfide. _Nano Lett._ 13, 2615–2622 (2013). CAS  Google Scholar  * Hong, J.

et al. Exploring atomic defects in molybdenum disulphide monolayers. _Nat. Commun._ 6, 6293 (2015). CAS  Google Scholar  * Vancsó, P. et al. The intrinsic defect structure of exfoliated MoS2

single layers revealed by scanning tunneling microscopy. _Sci. Rep._ 6, 29726 (2016). Google Scholar  * Edelberg, D. et al. Hundredfold enhancement of light emission via defect control in

monolayer transition-metal dichalcogenides. Preprint at https://arxiv.org/abs/1805.00127 (2018). * Zhang, S. et al. Defect structure of localized excitons in a WSe2 monolayer. _Phys. Rev.

Lett._ 119, 046101 (2017). Google Scholar  * Lin, Y.-C. et al. Realizing large-scale, electronic-grade two-dimensional semiconductors. _ACS Nano_ 12, 965–975 (2018). CAS  Google Scholar  *

Qiu, H. et al. Hopping transport through defect-induced localized states in molybdenum disulphide. _Nat. Commun._ 4, 2642 (2013). Google Scholar  * Gustafsson, M. V. et al. Ambipolar Landau

levels and strong band-selective carrier interactions in monolayer WSe2. _Nat. Mater._ 17, 411–415 (2018). CAS  Google Scholar  * Yu, Z. et al. Towards intrinsic charge transport in

monolayer molybdenum disulfide by defect and interface engineering. _Nat. Commun._ 5, 5290 (2014). CAS  Google Scholar  * Amani, M. et al. Near-unity photoluminescence quantum yield in MoS2.

_Science_ 350, 1065–1068 (2015). CAS  Google Scholar  * Addou, R. et al. Impurities and electronic property variations of natural MoS2 crystal surfaces. _ACS Nano_ 9, 9124–9133 (2015). CAS

  Google Scholar  * Addou, R. & Wallace, R. M. Surface analysis of WSe2 crystals: spatial and electronic variability. _ACS Appl. Mater. Interfaces_ 8, 26400–26406 (2016). CAS  Google

Scholar  * Das, S., Chen, H.-Y., Penumatcha, A. V. & Appenzeller, J. High performance multilayer MoS2 transistors with scandium contacts. _Nano Lett._ 13, 100–105 (2013). CAS  Google

Scholar  * Chuang, H.-J. et al. Low-resistance 2D/2D ohmic contacts: a universal approach to high- performance WSe2, MoS2, and MoSe2 transistors. _Nano Lett._ 16, 1896–1902 (2016). CAS 

Google Scholar  * Zhao, Y. et al. Doping, contact and interface engineering of two-dimensional layered transition metal dichalcogenides transistors. _Adv. Funct. Mater._ 27, 1603484 (2017).

Google Scholar  * He, Y.-M. et al. Single quantum emitters in monolayer semiconductors. _Nat. Nanotechnol._ 10, 497–502 (2015). CAS  Google Scholar  * Chakraborty, C., Kinnischtzke, L.,

Goodfellow, K. M., Beams, R. & Vamivakas, A. N. Voltage-controlled quantum light from an atomically thin semiconductor. _Nat. Nanotechnol._ 10, 507–511 (2015). CAS  Google Scholar  *

Tran, T. T., Bray, K., Ford, M. J., Toth, M. & Aharonovich, I. Quantum emission from hexagonal boron nitride monolayers. _Nat. Nanotechnol._ 11, 37–41 (2016). CAS  Google Scholar  *

Hinnemann, B. et al. Biomimetic hydrogen evolution: MoS2 nanoparticles as catalyst for hydrogen evolution. _J. Am. Chem. Soc._ 127, 5308–5309 (2005). CAS  Google Scholar  * Li, G. et al. All

the catalytic active sites of MoS2 for hydrogen evolution. _J. Am. Chem. Soc._ 138, 16632–16638 (2016). CAS  Google Scholar  * Guguchia, Z. et al. Magnetism in semiconducting molybdenum

dichalcogenides. _Sci. Adv._ 4, eaat3672 (2018). CAS  Google Scholar  * Zhang, J. et al. Magnetic molybdenum disulfide nanosheet films. _Nano Lett._ 7, 2370–2376 (2007). CAS  Google Scholar

  * Kaasbjerg, K., Martiny, J. H. J., Low, T. & Jauho, A.-P. Symmetry-forbidden intervalley scattering by atomic defects in monolayer transition-metal dichalcogenides. _Phys. Rev. B_ 96,

241411 (2017). Google Scholar  * Acerce, M., Voiry, D. & Chhowalla, M. Metallic 1T phase MoS2 nanosheets as supercapacitor electrode materials. _Nat. Nanotechnol._ 10, 313–318 (2015).

CAS  Google Scholar  * Kappera, R. et al. Phase-engineered low-resistance contacts for ultrathin MoS2 transistors. _Nat. Mater._ 13, 1128–1134 (2014). CAS  Google Scholar  * Kang, K. et al.

High-mobility three-atom-thick semiconducting films with wafer-scale homogeneity. _Nature_ 520, 656–660 (2015). CAS  Google Scholar  * Kang, K. et al. Layer-by-layer assembly of

two-dimensional materials into wafer-scale heterostructures. _Nature_ 550, 229–233 (2017). Google Scholar  * Shim, J. et al. Controlled crack propagation for atomic precision handling of

wafer-scale two-dimensional materials. _Science_ 362, 665–670 (2018). CAS  Google Scholar  * Jana, M. & Singh, R. N. Progress in CVD synthesis of layered hexagonal boron nitride with

tunable properties and their applications. _Int. Mater. Rev._ 63, 162–203 (2018). CAS  Google Scholar  * Kalantar-zadeh, K. et al. Two dimensional and layered transition metal oxides. _Appl.

Mater. Today_ 5, 73–89 (2016). Google Scholar  Download references ACKNOWLEDGEMENTS We would like to acknowledge M. Yankowitz and J. I. A. Li for many discussions involving graphene and

graphene devices. This work was supported the National Science Foundation Materials Research Science and Engineering Centers programme through Columbia in the Center for Precision Assembly

of Superstratic and Superatomic Solids (DMR-1420634). S.H.C. was supported by the Postdoctoral Research Program of Sungkyunkwan University (2016). AUTHOR INFORMATION Author notes * These

authors contributed equally: Daniel Rhodes, Sang Hoon Chae. AUTHORS AND AFFILIATIONS * Department of Mechanical Engineering, Columbia University, New York, NY, USA Daniel Rhodes, Sang Hoon

Chae & James Hone * Centre de Nanosciences et de Nanotechnologies (C2N), CNRS, Université Paris Sud, Université Paris-Saclay, Palaiseau, France Rebeca Ribeiro-Palau Authors * Daniel

Rhodes View author publications You can also search for this author inPubMed Google Scholar * Sang Hoon Chae View author publications You can also search for this author inPubMed Google

Scholar * Rebeca Ribeiro-Palau View author publications You can also search for this author inPubMed Google Scholar * James Hone View author publications You can also search for this author

inPubMed Google Scholar CORRESPONDING AUTHOR Correspondence to James Hone. ETHICS DECLARATIONS COMPETING INTERESTS The authors declare no competing interests. ADDITIONAL INFORMATION

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THIS ARTICLE CITE THIS ARTICLE Rhodes, D., Chae, S.H., Ribeiro-Palau, R. _et al._ Disorder in van der Waals heterostructures of 2D materials. _Nat. Mater._ 18, 541–549 (2019).

https://doi.org/10.1038/s41563-019-0366-8 Download citation * Received: 26 September 2018 * Accepted: 09 April 2019 * Published: 21 May 2019 * Issue Date: June 2019 * DOI:

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