Scalable Synthesis of Monolayer Hexagonal Boron Nitride on Graphene with Giant Bandgap Renormalization

Wang, Ping; Lee, Woncheol; Corbett, Joseph P.; Koll, William H.; Vu, Nguyen M.; Laleyan, David Arto; Wen, Qiannan; Wu, Yuanpeng; Pandey, Ayush; Gim, Jiseok; Wang, Ding; Qiu, Diana Y.; Hovden, Robert; Kira, Mackillo; Heron, John T.; Gupta, Jay A.; Kioupakis, Emmanouil; Mi, Zetian

doi:10.1002/adma.202201387

Title: Scalable Synthesis of Monolayer Hexagonal Boron Nitride on Graphene with Giant Bandgap Renormalization

Journal Article · Thu Apr 21 00:00:00 UTC 2022 · Advanced Materials

DOI: https://doi.org/10.1002/adma.202201387 · OSTI ID:1864058

^[1]; Lee, Woncheol ^[1]; Corbett, Joseph P. ^[2]; Koll, William H. ^[3]; Vu, Nguyen M. ^[4]; Laleyan, David Arto ^[1]; Wen, Qiannan ^[1]; Wu, Yuanpeng ^[1]; Pandey, Ayush ^[1]; Gim, Jiseok ^[4]; Wang, Ding ^[1]; Qiu, Diana Y. ^[5]; Hovden, Robert ^[4]; Kira, Mackillo ^[1]; Heron, John T. ^[4]; Gupta, Jay A. ^[3]; Kioupakis, Emmanouil ^[4]; Mi, Zetian ^[1]

Department of Electrical Engineering and Computer Science University of Michigan Ann Arbor MI 48109 USA
Department of Physics Ohio State University Columbus OH 43210 USA, UES Inc. 4401 Dayton‐Xenia Rd Dayton OH 45432 USA
Department of Physics Ohio State University Columbus OH 43210 USA
Department of Material Science and Engineering University of Michigan Ann Arbor MI 48109 USA
Department of Mechanical Engineering and Materials Science Yale University New Haven CT 06516 USA

Abstract Monolayer hexagonal boron nitride (hBN) has been widely considered a fundamental building block for 2D heterostructures and devices. However, the controlled and scalable synthesis of hBN and its 2D heterostructures has remained a daunting challenge. Here, an hBN/graphene (hBN/G) interface‐mediated growth process for the controlled synthesis of high‐quality monolayer hBN is proposed and further demonstrated. It is discovered that the in‐plane hBN/G interface can be precisely controlled, enabling the scalable epitaxy of unidirectional monolayer hBN on graphene, which exhibits a uniform moiré superlattice consistent with single‐domain hBN, aligned to the underlying graphene lattice. Furthermore, it is identified that the deep‐ultraviolet emission at 6.12 eV stems from the 1s‐exciton state of monolayer hBN with a giant renormalized direct bandgap on graphene. This work provides a viable path for the controlled synthesis of ultraclean, wafer‐scale, atomically ordered 2D quantum materials, as well as the fabrication of 2D quantum electronic and optoelectronic devices.

View Journal Article

Cite

Export

Save

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Yale Univ., New Haven, CT (United States)

Sponsoring Organization:: Kwanjeong Educational Foundation; National Science Foundation (NSF); US Army Research Office (ARO); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; W. M. Keck Foundation

Grant/Contract Number:: AC02-05CH11231; SC0021965

OSTI ID:: 1864058

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 21 Vol. 34; ISSN 0935-9648

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

References (57)

Graphene-Assisted Epitaxy of Nitrogen Lattice Polarity GaN Films on Non-Polar Sapphire Substrates for Green Light Emitting Diodes Liu, Fang; Zhang, Zhihong; Rong, Xin Advanced Functional Materials, Vol. 30, Issue 22 https://doi.org/10.1002/adfm.202001283	journal	March 2020
Epitaxial Growth of h‐BN on Templates of Various Dimensionalities in h‐BN–Graphene Material Systems Chen, Xin; Yang, He; Wu, Bin Advanced Materials, Vol. 31, Issue 12 https://doi.org/10.1002/adma.201805582	journal	January 2019
Synthesis of High‐Quality Graphene and Hexagonal Boron Nitride Monolayer In‐Plane Heterostructure on Cu–Ni Alloy Lu, Guangyuan; Wu, Tianru; Yang, Peng Advanced Science, Vol. 4, Issue 9 https://doi.org/10.1002/advs.201700076	journal	May 2017
Hexagonal BN‐Assisted Epitaxy of Strain Released GaN Films for True Green Light‐Emitting Diodes Liu, Fang; Yu, Ye; Zhang, Yuantao Advanced Science, Vol. 7, Issue 21 https://doi.org/10.1002/advs.202000917	journal	September 2020
Aligned Growth of Millimeter-Size Hexagonal Boron Nitride Single-Crystal Domains on Epitaxial Nickel Thin Film Meng, Junhua; Zhang, Xingwang; Wang, Ye Small, Vol. 13, Issue 18 https://doi.org/10.1002/smll.201604179	journal	March 2017
Oxide interfaces: pathways to novel phenomena Yu, Pu; Chu, Ying-Hao; Ramesh, Ramamoorthy Materials Today, Vol. 15, Issue 7-8 https://doi.org/10.1016/S1369-7021(12)70137-2	journal	July 2012
Structural and Electronic Properties of Interfaces in Graphene and Hexagonal Boron Nitride Lateral Heterostructures Zhang, Junfeng; Xie, Weiyu; Xu, Xiaohong Chemistry of Materials, Vol. 28, Issue 14 https://doi.org/10.1021/acs.chemmater.6b01764	journal	July 2016
Accelerating GW -Based Energy Level Alignment Calculations for Molecule–Metal Interfaces Using a Substrate Screening Approach Liu, Zhen-Fei; da Jornada, Felipe H.; Louie, Steven G. Journal of Chemical Theory and Computation, Vol. 15, Issue 7 https://doi.org/10.1021/acs.jctc.9b00326	journal	June 2019
Monolayer Boron Nitride: Hyperspectral Imaging in the Deep Ultraviolet Rousseau, Adrien; Ren, Lei; Durand, Alrik Nano Letters, Vol. 21, Issue 23 https://doi.org/10.1021/acs.nanolett.1c02531	journal	September 2021
Environmental Screening Effects in 2D Materials: Renormalization of the Bandgap, Electronic Structure, and Optical Spectra of Few-Layer Black Phosphorus Qiu, Diana Y.; da Jornada, Felipe H.; Louie, Steven G. Nano Letters, Vol. 17, Issue 8 https://doi.org/10.1021/acs.nanolett.7b01365	journal	July 2017
Highly Ordered Boron Nitride/Epigraphene Epitaxial Films on Silicon Carbide by Lateral Epitaxial Deposition Gigliotti, James; Li, Xin; Sundaram, Suresh ACS Nano, Vol. 14, Issue 10 https://doi.org/10.1021/acsnano.0c04164	journal	September 2020
Honeycomb Carbon: A Review of Graphene Allen, Matthew J.; Tung, Vincent C.; Kaner, Richard B. Chemical Reviews, Vol. 110, Issue 1, p. 132-145 https://doi.org/10.1021/cr900070d	journal	January 2010
Quantum Dots and Nanoroads of Graphene Embedded in Hexagonal Boron Nitride Bhowmick, Somnath; Singh, Abhishek K.; Yakobson, Boris I. The Journal of Physical Chemistry C, Vol. 115, Issue 20 https://doi.org/10.1021/jp200671p	journal	May 2011
Electron Tunneling through Ultrathin Boron Nitride Crystalline Barriers Britnell, Liam; Gorbachev, Roman V.; Jalil, Rashid Nano Letters, Vol. 12, Issue 3 https://doi.org/10.1021/nl3002205	journal	February 2012
Van der Waals heterostructures Geim, A. K.; Grigorieva, I. V. Nature, Vol. 499, Issue 7459, p. 419-425 https://doi.org/10.1038/nature12385	journal	July 2013
Direct-bandgap properties and evidence for ultraviolet lasing of hexagonal boron nitride single crystal Watanabe, Kenji; Taniguchi, Takashi; Kanda, Hisao Nature Materials, Vol. 3, Issue 6 https://doi.org/10.1038/nmat1134	journal	May 2004
Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor Ugeda, Miguel M.; Bradley, Aaron J.; Shi, Su-Fei Nature Materials, Vol. 13, Issue 12 https://doi.org/10.1038/nmat4061	journal	August 2014
Highly confined low-loss plasmons in graphene–boron nitride heterostructures Woessner, Achim; Lundeberg, Mark B.; Gao, Yuanda Nature Materials, Vol. 14, Issue 4 https://doi.org/10.1038/nmat4169	journal	December 2014
Stacked 2D materials shed light Wang, Xiaomu; Xia, Fengnian Nature Materials, Vol. 14, Issue 3 https://doi.org/10.1038/nmat4218	journal	February 2015
Isotope engineering of van der Waals interactions in hexagonal boron nitride Vuong, T. Q. P.; Liu, S.; Van der Lee, A. Nature Materials, Vol. 17, Issue 2 https://doi.org/10.1038/nmat5048	journal	December 2017
Hexagonal boron nitride is an indirect bandgap semiconductor Cassabois, G.; Valvin, P.; Gil, B. Nature Photonics, Vol. 10, Issue 4 https://doi.org/10.1038/nphoton.2015.277	journal	January 2016
Emergence of superlattice Dirac points in graphene on hexagonal boron nitride Yankowitz, Matthew; Xue, Jiamin; Cormode, Daniel Nature Physics, Vol. 8, Issue 5 https://doi.org/10.1038/nphys2272	journal	March 2012
Spin and valley quantum Hall ferromagnetism in graphene Young, A. F.; Dean, C. R.; Wang, L. Nature Physics, Vol. 8, Issue 7 https://doi.org/10.1038/nphys2307	journal	May 2012
Direct band-gap crossover in epitaxial monolayer boron nitride Elias, C.; Valvin, P.; Pelini, T. Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-10610-5	journal	June 2019
Epitaxial growth of a 100-square-centimetre single-crystal hexagonal boron nitride monolayer on copper Wang, Li; Xu, Xiaozhi; Zhang, Leining Nature, Vol. 570, Issue 7759 https://doi.org/10.1038/s41586-019-1226-z	journal	May 2019
Signatures of tunable superconductivity in a trilayer graphene moiré superlattice Chen, Guorui; Sharpe, Aaron L.; Gallagher, Patrick Nature, Vol. 572, Issue 7768 https://doi.org/10.1038/s41586-019-1393-y	journal	July 2019
Wafer-scale single-crystal hexagonal boron nitride monolayers on Cu (111) Chen, Tse-An; Chuu, Chih-Piao; Tseng, Chien-Chih Nature, Vol. 579, Issue 7798 https://doi.org/10.1038/s41586-020-2009-2	journal	March 2020
Interface effects in hybrid hBN-graphene nanoribbons Leon, Carlos; Costa, Marcio; Chico, Leonor Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-39763-5	journal	March 2019
Improvements in structural and optical properties of wafer-scale hexagonal boron nitride film by post-growth annealing Lee, Seung Hee; Jeong, Hokyeong; Okello, Odongo Francis Ngome Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-47093-9	journal	July 2019
van der Waals heterostructures combining graphene and hexagonal boron nitride Yankowitz, Matthew; Ma, Qiong; Jarillo-Herrero, Pablo Nature Reviews Physics, Vol. 1, Issue 2 https://doi.org/10.1038/s42254-018-0016-0	journal	January 2019
Hexagonal Boron Nitride Tunnel Barriers Grown on Graphite by High Temperature Molecular Beam Epitaxy Cho, Yong-Jin; Summerfield, Alex; Davies, Andrew Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep34474	journal	September 2016
Band gap engineering of graphene/ h -BN hybrid superlattices nanoribbons Li, Shilong; Ren, Zhaoyu; Zheng, Jiming Journal of Applied Physics, Vol. 113, Issue 3 https://doi.org/10.1063/1.4776208	journal	January 2013
Impact of the stacking sequence on the bandgap and luminescence properties of bulk, bilayer, and monolayer hexagonal boron nitride Mengle, K. A.; Kioupakis, E. APL Materials, Vol. 7, Issue 2 https://doi.org/10.1063/1.5087836	journal	February 2019
Strain-free ultrathin AlN epilayers grown directly on sapphire by high-temperature molecular beam epitaxy Laleyan, David Arto; Fernández-Delgado, Natalia; Reid, Eric T. Applied Physics Letters, Vol. 116, Issue 15 https://doi.org/10.1063/1.5144838	journal	April 2020
Graphene-assisted molecular beam epitaxy of AlN for AlGaN deep-ultraviolet light-emitting diodes Wang, Ping; Pandey, Ayush; Gim, Jiseok Applied Physics Letters, Vol. 116, Issue 17 https://doi.org/10.1063/1.5144906	journal	April 2020
Thermally annealed wafer-scale h-BN films grown on sapphire substrate by molecular beam epitaxy Liu, F.; Rong, X.; Yu, Y. Applied Physics Letters, Vol. 116, Issue 14 https://doi.org/10.1063/5.0002101	journal	April 2020
Four-inch high quality crack-free AlN layer grown on a high-temperature annealed AlN template by MOCVD Liu, Shangfeng; Yuan, Ye; Sheng, Shanshan Journal of Semiconductors, Vol. 42, Issue 12 https://doi.org/10.1088/1674-4926/42/12/122804	journal	December 2021
Interface engineering of electronic properties of graphene/boron nitride lateral heterostructures Zhang, Dong; Zhang, Dong-Bo; Yang, Fuhua 2D Materials, Vol. 2, Issue 4 https://doi.org/10.1088/2053-1583/2/4/041001	journal	November 2015
Direct determination of monolayer MoS ₂ and WSe ₂ exciton binding energies on insulating and metallic substrates Park, Soohyung; Mutz, Niklas; Schultz, Thorsten 2D Materials, Vol. 5, Issue 2 https://doi.org/10.1088/2053-1583/aaa4ca	journal	January 2018
Epitaxy of boron nitride monolayers for graphene-based lateral heterostructures Wrigley, James; Bradford, Jonathan; James, Tyler 2D Materials, Vol. 8, Issue 3 https://doi.org/10.1088/2053-1583/abea66	journal	March 2021
Band gap measurements of monolayer h-BN and insights into carbon-related point defects Román, Ricardo Javier Peña; Costa, Fábio J. R. Costa; Zobelli, Alberto 2D Materials, Vol. 8, Issue 4 https://doi.org/10.1088/2053-1583/ac0d9c	journal	July 2021
Exciton-polariton properties of hexagonal BN-based microcavity and their potential applications in BEC and superconductivity Yang, Huaiyuan; Wang, Xinqiang; Li, Xin-Zheng Physical Review B, Vol. 104, Issue 20 https://doi.org/10.1103/PhysRevB.104.205307	journal	November 2021
Intervalley scattering in hexagonal boron nitride Cassabois, G.; Valvin, P.; Gil, B. Physical Review B, Vol. 93, Issue 3 https://doi.org/10.1103/PhysRevB.93.035207	journal	January 2016
Excitons in boron nitride single layer Galvani, Thomas; Paleari, Fulvio; Miranda, Henrique P. C. Physical Review B, Vol. 94, Issue 12 https://doi.org/10.1103/PhysRevB.94.125303	journal	September 2016
Excitons in van der Waals materials: From monolayer to bulk hexagonal boron nitride Koskelo, Jaakko; Fugallo, Giorgia; Hakala, Mikko Physical Review B, Vol. 95, Issue 3 https://doi.org/10.1103/PhysRevB.95.035125	journal	January 2017
Theory of phonon-assisted luminescence in solids: Application to hexagonal boron nitride Cannuccia, E.; Monserrat, B.; Attaccalite, C. Physical Review B, Vol. 99, Issue 8 https://doi.org/10.1103/PhysRevB.99.081109	journal	February 2019
Giant exciton-phonon coupling and zero-point renormalization in hexagonal monolayer boron nitride Mishra, Himani; Bhattacharya, Sitangshu Physical Review B, Vol. 99, Issue 16 https://doi.org/10.1103/PhysRevB.99.165201	journal	April 2019
Direct Determination of Band-Gap Renormalization in the Photoexcited Monolayer MoS 2 Liu, Fang; Ziffer, Mark E.; Hansen, Kameron R. Physical Review Letters, Vol. 122, Issue 24 https://doi.org/10.1103/PhysRevLett.122.246803	journal	June 2019
Huge Excitonic Effects in Layered Hexagonal Boron Nitride Arnaud, B.; Lebègue, S.; Rabiller, P. Physical Review Letters, Vol. 96, Issue 2 https://doi.org/10.1103/PhysRevLett.96.026402	journal	January 2006
The electronic properties of graphene Castro Neto, A. H.; Guinea, F.; Peres, N. M. R. Reviews of Modern Physics, Vol. 81, Issue 1, p. 109-162 https://doi.org/10.1103/RevModPhys.81.109	journal	January 2009
Colloquium : Excitons in atomically thin transition metal dichalcogenides Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M. Reviews of Modern Physics, Vol. 90, Issue 2 https://doi.org/10.1103/RevModPhys.90.021001	journal	April 2018
Oxide Interfaces--An Opportunity for Electronics Mannhart, J.; Schlom, D. G. Science, Vol. 327, Issue 5973, p. 1607-1611 https://doi.org/10.1126/science.1181862	journal	March 2010
Evidence for a fractional fractal quantum Hall effect in graphene superlattices Wang, L.; Gao, Y.; Wen, B. Science, Vol. 350, Issue 6265 https://doi.org/10.1126/science.aad2102	journal	December 2015
Wafer-scale single-crystal hexagonal boron nitride film via self-collimated grain formation Lee, Joo Song; Choi, Soo Ho; Yun, Seok Joon Science, Vol. 362, Issue 6416 https://doi.org/10.1126/science.aau2132	journal	November 2018
Excitons in hexagonal boron nitride single-layer: a new platform for polaritonics in the ultraviolet Ferreira, F.; Chaves, A. J.; Peres, N. M. R. Journal of the Optical Society of America B, Vol. 36, Issue 3 https://doi.org/10.1364/JOSAB.36.000674	journal	January 2019
Effect of growth temperature on the structural and optical properties of few-layer hexagonal boron nitride by molecular beam epitaxy Laleyan, David Arto; Mengle, Kelsey; Zhao, Songrui Optics Express, Vol. 26, Issue 18 https://doi.org/10.1364/OE.26.023031	journal	January 2018
Low dislocation density AlN on sapphire prepared by double sputtering and annealing Wang, Ding; Uesugi, Kenjiro; Xiao, Shiyu Applied Physics Express, Vol. 13, Issue 9 https://doi.org/10.35848/1882-0786/ababec	journal	August 2020

Similar Records

Van der Waals epitaxial growth of two-dimensional single-crystalline GaSe domains on graphene

Journal Article · Wed Jul 22 00:00:00 UTC 2015 · ACS Nano · OSTI ID:1214495

Li, Xufan; Basile, Leonardo; Huang, Bing; +12 more

Two-dimensional heterostructures: fabrication, characterization, and application

Journal Article · Wed Aug 13 04:00:00 UTC 2014 · Nanoscale · OSTI ID:1286748

Wang, Hong; Liu, Fucai; Fu, Wei; +3 more

An outlook into the flat land of 2D materials beyond graphene: synthesis, properties and device applications

Journal Article · Tue Dec 01 00:00:00 UTC 2020 · 2D Materials · OSTI ID:1730955

McCreary, Amber; Kazakova, Olga; Jariwala, Deep; +1 more

Related Subjects

2D heterostructures
36 MATERIALS SCIENCE
bandgap
graphene
moiré superlattices
monolayer hexagonal boron nitride

Title: Scalable Synthesis of Monolayer Hexagonal Boron Nitride on Graphene with Giant Bandgap Renormalization

Citation Formats

References (57)

Similar Records

Related Subjects