Abstract

We have studied the epitaxy of few-layer hexagonal boron nitride (h-BN) by plasma-assisted molecular beam epitaxy (MBE) using a low growth rate and nitrogen-rich condition. It has been determined that under such conditions, the growth temperature is the factor having the most significant impact on the structural and optical quality of the material. When grown at temperatures <1000 °C, the h-BN film is polycrystalline, and defect-related photoluminescence (PL) emission dominates. Epitaxial domains of exceptional crystalline quality are obtained at elevated substrate temperatures of ~1300 °C, which exhibit strong band-edge PL emission at ~220 nm and negligible defect-related emission at room temperature. Our atomistic calculations reveal that, even though the gap of h-BN is indirect, it luminesces as strongly as direct-gap materials. Experimentally, the luminescence intensity of such a few-layer h-BN sample is measured to be two orders of magnitude stronger than that of a 4-µm thick commercially grown AlN template on sapphire, demonstrating the extraordinary potential of epitaxial h-BN for deep ultraviolet (UV) optoelectronics and quantum photonics.

© 2018 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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2018 (1)

I. Boulares, G. Shi, E. Kioupakis, P. Lošťák, C. Uher, and R. Merlin, “Surface phonons in the topological insulators Bi2Se3 and Bi2Te3,” Solid State Commun. 271, 1–5 (2018).
[Crossref]

2017 (12)

J. Meng, X. Zhang, Y. Wang, Z. Yin, H. Liu, J. Xia, H. Wang, J. You, P. Jin, D. Wang, and X.-M. Meng, “Aligned Growth of Millimeter-Size Hexagonal Boron Nitride Single-Crystal Domains on Epitaxial Nickel Thin Film,” Small 13(18), 1604179 (2017).
[Crossref] [PubMed]

J. M. Wofford, S. Nakhaie, T. Krause, X. Liu, M. Ramsteiner, M. Hanke, H. Riechert, and J. M. J Lopes, “A hybrid MBE-based growth method for large-area synthesis of stacked hexagonal boron nitride/graphene heterostructures,” Sci. Rep. 7, 43644 (2017).
[Crossref] [PubMed]

D. A. Laleyan, S. Zhao, S. Y. Woo, H. N. Tran, H. B. Le, T. Szkopek, H. Guo, G. A. Botton, and Z. Mi, “AlN/h-BN Heterostructures for Mg Dopant-Free Deep Ultraviolet Photonics,” Nano Lett. 17(6), 3738–3743 (2017).
[Crossref] [PubMed]

T. Q. P. Vuong, G. Cassabois, P. Valvin, V. Jacques, A. V. D. Lee, A. Zobelli, K. Watanabe, T. Taniguchi, and B. Gil, “Phonon symmetries in hexagonal boron nitride probed by incoherent light emission,” 2D Mater. 4, 011004 (2017).
[PubMed]

H. X. Jiang and J. Y. Lin, “Review—Hexagonal boron nitride epilayers: growth, optical properties and device applications,” ECS J. Solid State Sci. Technol. 6(2), Q3012–Q3021 (2017).
[Crossref]

N. Izyumskaya, D. O. Demchenko, S. Das, Ü. Özgür, V. Avrutin, and H. Morkoç, “Recent development of boron nitride towards electronic applications,” Adv. Electron. Mater. 3(5), 1600485 (2017).
[Crossref]

S. Sonde, A. Dolocan, N. Lu, C. Corbet, M. J. Kim, E. Tutuc, S. K. Banerjee, and L. Colombo, “Ultrathin, wafer-scale hexagonal boron nitride on dielectric surfaces by diffusion and segregation mechanism,” 2D Mater. 4(2), 025052 (2017).
[Crossref]

T. Q. P. Vuong, G. Cassabois, P. Valvin, E. Rousseau, A. Summerfield, C. J. Mellor, Y. Cho, T. S. Cheng, J. D. Albar, L. Eaves, C. T. Foxon, P. H. Beton, S. V. Novikov, and B. Gil, “Deep ultraviolet emission in hexagonal boron nitride grown by high-temperature molecular beam epitaxy,” 2D Mater. 4(2), 021023 (2017).
[Crossref]

F. Mahvash, S. Eissa, T. Bordjiba, A. C. Tavares, T. Szkopek, and M. Siaj, “Corrosion resistance of monolayer hexagonal boron nitride on copper,” Sci. Rep. 7(1), 42139 (2017).
[Crossref] [PubMed]

K. Ahmed, R. Dahal, A. Weltz, J. J.-Q. Lu, Y. Danon, and I. B. Bhat, “Effects of sapphire nitridation and growth temperature on the epitaxial growth of hexagonal boron nitride on sapphire,” Mater. Res. Express 4(1), 015007 (2017).
[Crossref]

Z. Xu, H. Tian, A. Khanaki, R. Zheng, M. Suja, and J. Liu, “Large-area growth of multi-layer hexagonal boron nitride on polished cobalt foils by plasma-assisted molecular beam epitaxy,” Sci. Rep. 7(1), 43100 (2017).
[Crossref] [PubMed]

I. Stenger, L. Schué, M. Boukhicha, B. Berini, B. Plaçais, A. Loiseau, and J. Barjon, “Low frequency Raman spectroscopy of few-atomic-layer thick hBN crystals,” 2D Mater. 4(3), 031003 (2017).
[Crossref]

2016 (8)

A.-R. Jang, S. Hong, C. Hyun, S. I. Yoon, G. Kim, H. Y. Jeong, T. J. Shin, S. O. Park, K. Wong, S. K. Kwak, N. Park, K. Yu, E. Choi, A. Mishchenko, F. Withers, K. S. Novoselov, H. Lim, and H. S. Shin, “Wafer-scale and wrinkle-free epitaxial growth of single-oriented multilayer hexagonal boron nitride on sapphire,” Nano Lett. 16(5), 3360–3366 (2016).
[Crossref] [PubMed]

A. A. Tonkikh, E. N. Voloshina, P. Werner, H. Blumtritt, B. Senkovskiy, G. Güntherodt, S. S. P. Parkin, and Y. S. Dedkov, “Structural and electronic properties of epitaxial multilayer h-BN on Ni(111) for spintronics applications,” Sci. Rep. 6(1), 23547 (2016).
[Crossref] [PubMed]

Y.-J. Cho, A. Summerfield, A. Davies, T. S. Cheng, E. F. Smith, C. J. Mellor, A. N. Khlobystov, C. T. Foxon, L. Eaves, P. H. Beton, and S. V. Novikov, “Hexagonal Boron Nitride Tunnel Barriers Grown on Graphite by High Temperature Molecular Beam Epitaxy,” Sci. Rep. 6(1), 34474 (2016).
[Crossref] [PubMed]

X. Z. Du, J. Li, J. Y. Lin, and H. X. Jiang, “The origins of near band-edge transitions in hexagonal boron nitride epilayers,” Appl. Phys. Lett. 108(5), 052106 (2016).
[Crossref]

K. Ahmed, R. Dahal, A. Weltz, J.-Q. Lu, Y. Danon, and I. B. Bhat, “Growth of hexagonal boron nitride on (111) Si for deep UV photonics and thermal neutron detection,” Appl. Phys. Lett. 109(11), 113501 (2016).
[Crossref]

J. Li, X. K. Cao, T. B. Hoffman, J. H. Edgar, J. Y. Lin, and H. X. Jiang, “Nature of exciton transitions in hexagonal boron nitride,” Appl. Phys. Lett. 108(12), 122101 (2016).
[Crossref]

T. C. Doan, J. Li, J. Y. Lin, and H. X. Jiang, “Bandgap and exciton binding energies of hexagonal boron nitride probed by photocurrent excitation spectroscopy,” Appl. Phys. Lett. 109(12), 122101 (2016).
[Crossref]

G. Cassabois, P. Valvin, and B. Gil, “Hexagonal boron nitride is an indirect bandgap semiconductor,” Nat. Photonics 10(4), 262–266 (2016).
[Crossref]

2015 (7)

Z. Xu, R. Zheng, A. Khanaki, Z. Zuo, and J. Liu, “Direct growth of graphene on in situ epitaxial hexagonal boron nitride flakes by plasma-assisted molecular beam epitaxy,” Appl. Phys. Lett. 107(21), 213103 (2015).
[Crossref]

S. Nakhaie, J. M. Wofford, T. Schumann, U. Jahn, M. Ramsteiner, M. Hanke, J. M. J. Lopes, and H. Riechert, “Synthesis of atomically thin hexagonal boron nitride films on nickel foils by molecular beam epitaxy,” Appl. Phys. Lett. 106(21), 213108 (2015).
[Crossref]

H. Wang, X. Zhang, H. Liu, Z. Yin, J. Meng, J. Xia, X.-M. Meng, J. Wu, and J. You, “Synthesis of Large-Sized Single-Crystal Hexagonal Boron Nitride Domains on Nickel Foils by Ion Beam Sputtering Deposition,” Adv. Mater. 27(48), 8109–8115 (2015).
[Crossref] [PubMed]

J. M. Rondinelli and E. Kioupakis, “Predicting and Designing Optical Properties of Inorganic Materials,” Annu. Rev. Mater. Res. 45(1), 491–518 (2015).
[Crossref]

G. Lu, T. Wu, Q. Yuan, H. Wang, H. Wang, F. Ding, X. Xie, and M. Jiang, “Synthesis of large single-crystal hexagonal boron nitride grains on Cu-Ni alloy,” Nat. Commun. 6(1), 6160 (2015).
[Crossref] [PubMed]

H. Peelaers, E. Kioupakis, and C. G. Van de Walle, “Free-carrier absorption in transparent conducting oxides: Phonon and impurity scattering in SnO2,” Phys. Rev. B 92(23), 235201 (2015).
[Crossref]

G. Shi and E. Kioupakis, “Electronic and Optical Properties of Nanoporous Silicon for Solar-Cell Applications,” ACS Photonics 2(2), 208–215 (2015).
[Crossref]

2014 (3)

J.-H. Park, J. C. Park, S. J. Yun, H. Kim, D. H. Luong, S. M. Kim, S. H. Choi, W. Yang, J. Kong, K. K. Kim, and Y. H. Lee, “Large-Area Monolayer Hexagonal Boron Nitride on Pt Foil,” ACS Nano 8(8), 8520–8528 (2014).
[Crossref] [PubMed]

H. X. Jiang and J. Y. Lin, “Hexagonal boron nitride for deep ultraviolet photonic devices,” Semicond. Sci. Technol. 29(8), 084003 (2014).
[Crossref]

A. Pakdel, Y. Bando, and D. Golberg, “Nano boron nitride flatland,” Chem. Soc. Rev. 43(3), 934–959 (2014).
[Crossref] [PubMed]

2013 (2)

A. K. Geim and I. V. Grigorieva, “Van der Waals heterostructures,” Nature 499(7459), 419–425 (2013).
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Z. Liu, Y. Gong, W. Zhou, L. Ma, J. Yu, J. C. Idrobo, J. Jung, A. H. MacDonald, R. Vajtai, J. Lou, and P. M. Ajayan, “Ultrathin high-temperature oxidation-resistant coatings of hexagonal boron nitride,” Nat. Commun. 4(1), 2541 (2013).
[Crossref] [PubMed]

2012 (4)

K. K. Kim, A. Hsu, X. Jia, S. M. Kim, Y. Shi, M. Hofmann, D. Nezich, J. F. Rodriguez-Nieva, M. Dresselhaus, T. Palacios, and J. Kong, “Synthesis of Monolayer Hexagonal Boron Nitride on Cu Foil Using Chemical Vapor Deposition,” Nano Lett. 12(1), 161–166 (2012).
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J. Noffsinger, E. Kioupakis, C. G. Van de Walle, S. G. Louie, and M. L. Cohen, “Phonon-Assisted Optical Absorption in Silicon from First Principles,” Phys. Rev. Lett. 108(16), 167402 (2012).
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J. Deslippe, G. Samsonidze, D. A. Strubbe, M. Jain, M. L. Cohen, and S. G. Louie, “BerkeleyGW: A massively parallel computer package for the calculation of the quasiparticle and optical properties of materials and nanostructures,” Comput. Phys. Commun. 183(6), 1269–1289 (2012).
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N. Marzari, A. A. Mostofi, J. R. Yates, I. Souza, and D. Vanderbilt, “Maximally localized Wannier functions: Theory and applications,” Rev. Mod. Phys. 84(4), 1419–1475 (2012).
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2011 (1)

R. V. Gorbachev, I. Riaz, R. R. Nair, R. Jalil, L. Britnell, B. D. Belle, E. W. Hill, K. S. Novoselov, K. Watanabe, T. Taniguchi, A. K. Geim, and P. Blake, “Hunting for Monolayer Boron Nitride: Optical and Raman Signatures,” Small 7(4), 465–468 (2011).
[Crossref] [PubMed]

2010 (3)

L. Song, L. Ci, H. Lu, P. B. Sorokin, C. Jin, J. Ni, A. G. Kvashnin, D. G. Kvashnin, J. Lou, B. I. Yakobson, and P. M. Ajayan, “Large Scale Growth and Characterization of Atomic Hexagonal Boron Nitride Layers,” Nano Lett. 10(8), 3209–3215 (2010).
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Y. Kobayashi, C.-L. Tsai, and T. Akasaka, “Optical band gap of h-BN epitaxial film grown on c -plane sapphire substrate,” Phys. Status Solidi., C Curr. Top. Solid State Phys. 7(7-8), 1906–1908 (2010).
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Y. Shi, C. Hamsen, X. Jia, K. K. Kim, A. Reina, M. Hofmann, A. L. Hsu, K. Zhang, H. Li, Z.-Y. Juang, M. S. Dresselhaus, L.-J. Li, and J. Kong, “Synthesis of Few-Layer Hexagonal Boron Nitride Thin Film by Chemical Vapor Deposition,” Nano Lett. 10(10), 4134–4139 (2010).
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2009 (2)

C. L. Tsai, Y. Kobayashi, T. Akasaka, and M. Kasu, “Molecular beam epitaxial growth of hexagonal boron nitride on Ni(1 1 1) substrate,” J. Cryst. Growth 311(10), 3054–3057 (2009).
[Crossref]

P. Giannozzi, S. Baroni, N. Bonini, M. Calandra, R. Car, C. Cavazzoni, D. Ceresoli, G. L. Chiarotti, M. Cococcioni, I. Dabo, A. Dal Corso, S. de Gironcoli, S. Fabris, G. Fratesi, R. Gebauer, U. Gerstmann, C. Gougoussis, A. Kokalj, M. Lazzeri, L. Martin-Samos, N. Marzari, F. Mauri, R. Mazzarello, S. Paolini, A. Pasquarello, L. Paulatto, C. Sbraccia, S. Scandolo, G. Sclauzero, A. P. Seitsonen, A. Smogunov, P. Umari, and R. M. Wentzcovitch, “QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials,” J. Phys. Condens. Matter 21(39), 395502 (2009).
[Crossref] [PubMed]

2008 (1)

A. A. Mostofi, J. R. Yates, Y.-S. Lee, I. Souza, D. Vanderbilt, and N. Marzari, “wannier90: a tool for obtaining maximally-localised Wannier functions,” Comput. Phys. Commun. 178(9), 685–699 (2008).
[Crossref]

2007 (2)

J. Serrano, A. Bosak, R. Arenal, M. Krisch, K. Watanabe, T. Taniguchi, H. Kanda, A. Rubio, and L. Wirtz, “Vibrational Properties of Hexagonal Boron Nitride: Inelastic X-Ray Scattering and ab Initio Calculations,” Phys. Rev. Lett. 98(9), 095503 (2007).
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F. Tang, T. Parker, G.-C. Wang, and T.-M. Lu, “Surface texture evolution of polycrystalline and nanostructured films: RHEED surface pole figure analysis,” J. Phys. Appl. Phys. 40(23), R427–R439 (2007).
[Crossref]

2005 (2)

S. Reich, A. C. Ferrari, R. Arenal, A. Loiseau, I. Bello, and J. Robertson, “Resonant Raman scattering in cubic and hexagonal boron nitride,” Phys. Rev. B 71(20), 205201 (2005).
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A. Preobrajenski, A. Vinogradov, and N. Mårtensson, “Monolayer of h-BN chemisorbed on Cu(111) and Ni(111): The role of the transition metal 3d states,” Surf. Sci. 582(1-3), 21–30 (2005).
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2004 (2)

W. Auwärter, H. U. Suter, H. Sachdev, and T. Greber, “Synthesis of One Monolayer of Hexagonal Boron Nitride on Ni(111) from B-Trichloroborazine (ClBNH)3,” Chem. Mater. 16(2), 343–345 (2004).
[Crossref]

K. Watanabe, T. Taniguchi, and H. Kanda, “Direct-bandgap properties and evidence for ultraviolet lasing of hexagonal boron nitride single crystal,” Nat. Mater. 3(6), 404–409 (2004).
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2001 (1)

S. Baroni, S. de Gironcoli, A. Dal Corso, and P. Giannozzi, “Phonons and related crystal properties from density-functional perturbation theory,” Rev. Mod. Phys. 73(2), 515–562 (2001).
[Crossref]

1998 (1)

H. Okumura, K. Balakrishnan, H. Hamaguchi, S. Takayoshi Koizumi, S. Chichibu, H. Nakanishi, T. Nagatomo, and S. Yoshida, “Analysis of MBE growth mode for GaN epilayers by RHEED,” J. Cryst. Growth 189–190, 364–369 (1998).
[Crossref]

Ahmed, K.

K. Ahmed, R. Dahal, A. Weltz, J. J.-Q. Lu, Y. Danon, and I. B. Bhat, “Effects of sapphire nitridation and growth temperature on the epitaxial growth of hexagonal boron nitride on sapphire,” Mater. Res. Express 4(1), 015007 (2017).
[Crossref]

K. Ahmed, R. Dahal, A. Weltz, J.-Q. Lu, Y. Danon, and I. B. Bhat, “Growth of hexagonal boron nitride on (111) Si for deep UV photonics and thermal neutron detection,” Appl. Phys. Lett. 109(11), 113501 (2016).
[Crossref]

Ajayan, P. M.

Z. Liu, Y. Gong, W. Zhou, L. Ma, J. Yu, J. C. Idrobo, J. Jung, A. H. MacDonald, R. Vajtai, J. Lou, and P. M. Ajayan, “Ultrathin high-temperature oxidation-resistant coatings of hexagonal boron nitride,” Nat. Commun. 4(1), 2541 (2013).
[Crossref] [PubMed]

L. Song, L. Ci, H. Lu, P. B. Sorokin, C. Jin, J. Ni, A. G. Kvashnin, D. G. Kvashnin, J. Lou, B. I. Yakobson, and P. M. Ajayan, “Large Scale Growth and Characterization of Atomic Hexagonal Boron Nitride Layers,” Nano Lett. 10(8), 3209–3215 (2010).
[Crossref] [PubMed]

Akasaka, T.

Y. Kobayashi, C.-L. Tsai, and T. Akasaka, “Optical band gap of h-BN epitaxial film grown on c -plane sapphire substrate,” Phys. Status Solidi., C Curr. Top. Solid State Phys. 7(7-8), 1906–1908 (2010).
[Crossref]

C. L. Tsai, Y. Kobayashi, T. Akasaka, and M. Kasu, “Molecular beam epitaxial growth of hexagonal boron nitride on Ni(1 1 1) substrate,” J. Cryst. Growth 311(10), 3054–3057 (2009).
[Crossref]

Albar, J. D.

T. Q. P. Vuong, G. Cassabois, P. Valvin, E. Rousseau, A. Summerfield, C. J. Mellor, Y. Cho, T. S. Cheng, J. D. Albar, L. Eaves, C. T. Foxon, P. H. Beton, S. V. Novikov, and B. Gil, “Deep ultraviolet emission in hexagonal boron nitride grown by high-temperature molecular beam epitaxy,” 2D Mater. 4(2), 021023 (2017).
[Crossref]

Arenal, R.

J. Serrano, A. Bosak, R. Arenal, M. Krisch, K. Watanabe, T. Taniguchi, H. Kanda, A. Rubio, and L. Wirtz, “Vibrational Properties of Hexagonal Boron Nitride: Inelastic X-Ray Scattering and ab Initio Calculations,” Phys. Rev. Lett. 98(9), 095503 (2007).
[Crossref] [PubMed]

S. Reich, A. C. Ferrari, R. Arenal, A. Loiseau, I. Bello, and J. Robertson, “Resonant Raman scattering in cubic and hexagonal boron nitride,” Phys. Rev. B 71(20), 205201 (2005).
[Crossref]

Auwärter, W.

W. Auwärter, H. U. Suter, H. Sachdev, and T. Greber, “Synthesis of One Monolayer of Hexagonal Boron Nitride on Ni(111) from B-Trichloroborazine (ClBNH)3,” Chem. Mater. 16(2), 343–345 (2004).
[Crossref]

Avrutin, V.

N. Izyumskaya, D. O. Demchenko, S. Das, Ü. Özgür, V. Avrutin, and H. Morkoç, “Recent development of boron nitride towards electronic applications,” Adv. Electron. Mater. 3(5), 1600485 (2017).
[Crossref]

Balakrishnan, K.

H. Okumura, K. Balakrishnan, H. Hamaguchi, S. Takayoshi Koizumi, S. Chichibu, H. Nakanishi, T. Nagatomo, and S. Yoshida, “Analysis of MBE growth mode for GaN epilayers by RHEED,” J. Cryst. Growth 189–190, 364–369 (1998).
[Crossref]

Bando, Y.

A. Pakdel, Y. Bando, and D. Golberg, “Nano boron nitride flatland,” Chem. Soc. Rev. 43(3), 934–959 (2014).
[Crossref] [PubMed]

Banerjee, S. K.

S. Sonde, A. Dolocan, N. Lu, C. Corbet, M. J. Kim, E. Tutuc, S. K. Banerjee, and L. Colombo, “Ultrathin, wafer-scale hexagonal boron nitride on dielectric surfaces by diffusion and segregation mechanism,” 2D Mater. 4(2), 025052 (2017).
[Crossref]

Barjon, J.

I. Stenger, L. Schué, M. Boukhicha, B. Berini, B. Plaçais, A. Loiseau, and J. Barjon, “Low frequency Raman spectroscopy of few-atomic-layer thick hBN crystals,” 2D Mater. 4(3), 031003 (2017).
[Crossref]

Baroni, S.

P. Giannozzi, S. Baroni, N. Bonini, M. Calandra, R. Car, C. Cavazzoni, D. Ceresoli, G. L. Chiarotti, M. Cococcioni, I. Dabo, A. Dal Corso, S. de Gironcoli, S. Fabris, G. Fratesi, R. Gebauer, U. Gerstmann, C. Gougoussis, A. Kokalj, M. Lazzeri, L. Martin-Samos, N. Marzari, F. Mauri, R. Mazzarello, S. Paolini, A. Pasquarello, L. Paulatto, C. Sbraccia, S. Scandolo, G. Sclauzero, A. P. Seitsonen, A. Smogunov, P. Umari, and R. M. Wentzcovitch, “QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials,” J. Phys. Condens. Matter 21(39), 395502 (2009).
[Crossref] [PubMed]

S. Baroni, S. de Gironcoli, A. Dal Corso, and P. Giannozzi, “Phonons and related crystal properties from density-functional perturbation theory,” Rev. Mod. Phys. 73(2), 515–562 (2001).
[Crossref]

Belle, B. D.

R. V. Gorbachev, I. Riaz, R. R. Nair, R. Jalil, L. Britnell, B. D. Belle, E. W. Hill, K. S. Novoselov, K. Watanabe, T. Taniguchi, A. K. Geim, and P. Blake, “Hunting for Monolayer Boron Nitride: Optical and Raman Signatures,” Small 7(4), 465–468 (2011).
[Crossref] [PubMed]

Bello, I.

S. Reich, A. C. Ferrari, R. Arenal, A. Loiseau, I. Bello, and J. Robertson, “Resonant Raman scattering in cubic and hexagonal boron nitride,” Phys. Rev. B 71(20), 205201 (2005).
[Crossref]

Berini, B.

I. Stenger, L. Schué, M. Boukhicha, B. Berini, B. Plaçais, A. Loiseau, and J. Barjon, “Low frequency Raman spectroscopy of few-atomic-layer thick hBN crystals,” 2D Mater. 4(3), 031003 (2017).
[Crossref]

Beton, P. H.

T. Q. P. Vuong, G. Cassabois, P. Valvin, E. Rousseau, A. Summerfield, C. J. Mellor, Y. Cho, T. S. Cheng, J. D. Albar, L. Eaves, C. T. Foxon, P. H. Beton, S. V. Novikov, and B. Gil, “Deep ultraviolet emission in hexagonal boron nitride grown by high-temperature molecular beam epitaxy,” 2D Mater. 4(2), 021023 (2017).
[Crossref]

Y.-J. Cho, A. Summerfield, A. Davies, T. S. Cheng, E. F. Smith, C. J. Mellor, A. N. Khlobystov, C. T. Foxon, L. Eaves, P. H. Beton, and S. V. Novikov, “Hexagonal Boron Nitride Tunnel Barriers Grown on Graphite by High Temperature Molecular Beam Epitaxy,” Sci. Rep. 6(1), 34474 (2016).
[Crossref] [PubMed]

Bhat, I. B.

K. Ahmed, R. Dahal, A. Weltz, J. J.-Q. Lu, Y. Danon, and I. B. Bhat, “Effects of sapphire nitridation and growth temperature on the epitaxial growth of hexagonal boron nitride on sapphire,” Mater. Res. Express 4(1), 015007 (2017).
[Crossref]

K. Ahmed, R. Dahal, A. Weltz, J.-Q. Lu, Y. Danon, and I. B. Bhat, “Growth of hexagonal boron nitride on (111) Si for deep UV photonics and thermal neutron detection,” Appl. Phys. Lett. 109(11), 113501 (2016).
[Crossref]

Blake, P.

R. V. Gorbachev, I. Riaz, R. R. Nair, R. Jalil, L. Britnell, B. D. Belle, E. W. Hill, K. S. Novoselov, K. Watanabe, T. Taniguchi, A. K. Geim, and P. Blake, “Hunting for Monolayer Boron Nitride: Optical and Raman Signatures,” Small 7(4), 465–468 (2011).
[Crossref] [PubMed]

Blumtritt, H.

A. A. Tonkikh, E. N. Voloshina, P. Werner, H. Blumtritt, B. Senkovskiy, G. Güntherodt, S. S. P. Parkin, and Y. S. Dedkov, “Structural and electronic properties of epitaxial multilayer h-BN on Ni(111) for spintronics applications,” Sci. Rep. 6(1), 23547 (2016).
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Bonini, N.

P. Giannozzi, S. Baroni, N. Bonini, M. Calandra, R. Car, C. Cavazzoni, D. Ceresoli, G. L. Chiarotti, M. Cococcioni, I. Dabo, A. Dal Corso, S. de Gironcoli, S. Fabris, G. Fratesi, R. Gebauer, U. Gerstmann, C. Gougoussis, A. Kokalj, M. Lazzeri, L. Martin-Samos, N. Marzari, F. Mauri, R. Mazzarello, S. Paolini, A. Pasquarello, L. Paulatto, C. Sbraccia, S. Scandolo, G. Sclauzero, A. P. Seitsonen, A. Smogunov, P. Umari, and R. M. Wentzcovitch, “QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials,” J. Phys. Condens. Matter 21(39), 395502 (2009).
[Crossref] [PubMed]

Bordjiba, T.

F. Mahvash, S. Eissa, T. Bordjiba, A. C. Tavares, T. Szkopek, and M. Siaj, “Corrosion resistance of monolayer hexagonal boron nitride on copper,” Sci. Rep. 7(1), 42139 (2017).
[Crossref] [PubMed]

Bosak, A.

J. Serrano, A. Bosak, R. Arenal, M. Krisch, K. Watanabe, T. Taniguchi, H. Kanda, A. Rubio, and L. Wirtz, “Vibrational Properties of Hexagonal Boron Nitride: Inelastic X-Ray Scattering and ab Initio Calculations,” Phys. Rev. Lett. 98(9), 095503 (2007).
[Crossref] [PubMed]

Botton, G. A.

D. A. Laleyan, S. Zhao, S. Y. Woo, H. N. Tran, H. B. Le, T. Szkopek, H. Guo, G. A. Botton, and Z. Mi, “AlN/h-BN Heterostructures for Mg Dopant-Free Deep Ultraviolet Photonics,” Nano Lett. 17(6), 3738–3743 (2017).
[Crossref] [PubMed]

Boukhicha, M.

I. Stenger, L. Schué, M. Boukhicha, B. Berini, B. Plaçais, A. Loiseau, and J. Barjon, “Low frequency Raman spectroscopy of few-atomic-layer thick hBN crystals,” 2D Mater. 4(3), 031003 (2017).
[Crossref]

Boulares, I.

I. Boulares, G. Shi, E. Kioupakis, P. Lošťák, C. Uher, and R. Merlin, “Surface phonons in the topological insulators Bi2Se3 and Bi2Te3,” Solid State Commun. 271, 1–5 (2018).
[Crossref]

Britnell, L.

R. V. Gorbachev, I. Riaz, R. R. Nair, R. Jalil, L. Britnell, B. D. Belle, E. W. Hill, K. S. Novoselov, K. Watanabe, T. Taniguchi, A. K. Geim, and P. Blake, “Hunting for Monolayer Boron Nitride: Optical and Raman Signatures,” Small 7(4), 465–468 (2011).
[Crossref] [PubMed]

Calandra, M.

P. Giannozzi, S. Baroni, N. Bonini, M. Calandra, R. Car, C. Cavazzoni, D. Ceresoli, G. L. Chiarotti, M. Cococcioni, I. Dabo, A. Dal Corso, S. de Gironcoli, S. Fabris, G. Fratesi, R. Gebauer, U. Gerstmann, C. Gougoussis, A. Kokalj, M. Lazzeri, L. Martin-Samos, N. Marzari, F. Mauri, R. Mazzarello, S. Paolini, A. Pasquarello, L. Paulatto, C. Sbraccia, S. Scandolo, G. Sclauzero, A. P. Seitsonen, A. Smogunov, P. Umari, and R. M. Wentzcovitch, “QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials,” J. Phys. Condens. Matter 21(39), 395502 (2009).
[Crossref] [PubMed]

Cao, X. K.

J. Li, X. K. Cao, T. B. Hoffman, J. H. Edgar, J. Y. Lin, and H. X. Jiang, “Nature of exciton transitions in hexagonal boron nitride,” Appl. Phys. Lett. 108(12), 122101 (2016).
[Crossref]

Car, R.

P. Giannozzi, S. Baroni, N. Bonini, M. Calandra, R. Car, C. Cavazzoni, D. Ceresoli, G. L. Chiarotti, M. Cococcioni, I. Dabo, A. Dal Corso, S. de Gironcoli, S. Fabris, G. Fratesi, R. Gebauer, U. Gerstmann, C. Gougoussis, A. Kokalj, M. Lazzeri, L. Martin-Samos, N. Marzari, F. Mauri, R. Mazzarello, S. Paolini, A. Pasquarello, L. Paulatto, C. Sbraccia, S. Scandolo, G. Sclauzero, A. P. Seitsonen, A. Smogunov, P. Umari, and R. M. Wentzcovitch, “QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials,” J. Phys. Condens. Matter 21(39), 395502 (2009).
[Crossref] [PubMed]

Cassabois, G.

T. Q. P. Vuong, G. Cassabois, P. Valvin, V. Jacques, A. V. D. Lee, A. Zobelli, K. Watanabe, T. Taniguchi, and B. Gil, “Phonon symmetries in hexagonal boron nitride probed by incoherent light emission,” 2D Mater. 4, 011004 (2017).
[PubMed]

T. Q. P. Vuong, G. Cassabois, P. Valvin, E. Rousseau, A. Summerfield, C. J. Mellor, Y. Cho, T. S. Cheng, J. D. Albar, L. Eaves, C. T. Foxon, P. H. Beton, S. V. Novikov, and B. Gil, “Deep ultraviolet emission in hexagonal boron nitride grown by high-temperature molecular beam epitaxy,” 2D Mater. 4(2), 021023 (2017).
[Crossref]

G. Cassabois, P. Valvin, and B. Gil, “Hexagonal boron nitride is an indirect bandgap semiconductor,” Nat. Photonics 10(4), 262–266 (2016).
[Crossref]

Cavazzoni, C.

P. Giannozzi, S. Baroni, N. Bonini, M. Calandra, R. Car, C. Cavazzoni, D. Ceresoli, G. L. Chiarotti, M. Cococcioni, I. Dabo, A. Dal Corso, S. de Gironcoli, S. Fabris, G. Fratesi, R. Gebauer, U. Gerstmann, C. Gougoussis, A. Kokalj, M. Lazzeri, L. Martin-Samos, N. Marzari, F. Mauri, R. Mazzarello, S. Paolini, A. Pasquarello, L. Paulatto, C. Sbraccia, S. Scandolo, G. Sclauzero, A. P. Seitsonen, A. Smogunov, P. Umari, and R. M. Wentzcovitch, “QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials,” J. Phys. Condens. Matter 21(39), 395502 (2009).
[Crossref] [PubMed]

Ceresoli, D.

P. Giannozzi, S. Baroni, N. Bonini, M. Calandra, R. Car, C. Cavazzoni, D. Ceresoli, G. L. Chiarotti, M. Cococcioni, I. Dabo, A. Dal Corso, S. de Gironcoli, S. Fabris, G. Fratesi, R. Gebauer, U. Gerstmann, C. Gougoussis, A. Kokalj, M. Lazzeri, L. Martin-Samos, N. Marzari, F. Mauri, R. Mazzarello, S. Paolini, A. Pasquarello, L. Paulatto, C. Sbraccia, S. Scandolo, G. Sclauzero, A. P. Seitsonen, A. Smogunov, P. Umari, and R. M. Wentzcovitch, “QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials,” J. Phys. Condens. Matter 21(39), 395502 (2009).
[Crossref] [PubMed]

Cheng, T. S.

T. Q. P. Vuong, G. Cassabois, P. Valvin, E. Rousseau, A. Summerfield, C. J. Mellor, Y. Cho, T. S. Cheng, J. D. Albar, L. Eaves, C. T. Foxon, P. H. Beton, S. V. Novikov, and B. Gil, “Deep ultraviolet emission in hexagonal boron nitride grown by high-temperature molecular beam epitaxy,” 2D Mater. 4(2), 021023 (2017).
[Crossref]

Y.-J. Cho, A. Summerfield, A. Davies, T. S. Cheng, E. F. Smith, C. J. Mellor, A. N. Khlobystov, C. T. Foxon, L. Eaves, P. H. Beton, and S. V. Novikov, “Hexagonal Boron Nitride Tunnel Barriers Grown on Graphite by High Temperature Molecular Beam Epitaxy,” Sci. Rep. 6(1), 34474 (2016).
[Crossref] [PubMed]

Chiarotti, G. L.

P. Giannozzi, S. Baroni, N. Bonini, M. Calandra, R. Car, C. Cavazzoni, D. Ceresoli, G. L. Chiarotti, M. Cococcioni, I. Dabo, A. Dal Corso, S. de Gironcoli, S. Fabris, G. Fratesi, R. Gebauer, U. Gerstmann, C. Gougoussis, A. Kokalj, M. Lazzeri, L. Martin-Samos, N. Marzari, F. Mauri, R. Mazzarello, S. Paolini, A. Pasquarello, L. Paulatto, C. Sbraccia, S. Scandolo, G. Sclauzero, A. P. Seitsonen, A. Smogunov, P. Umari, and R. M. Wentzcovitch, “QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials,” J. Phys. Condens. Matter 21(39), 395502 (2009).
[Crossref] [PubMed]

Chichibu, S.

H. Okumura, K. Balakrishnan, H. Hamaguchi, S. Takayoshi Koizumi, S. Chichibu, H. Nakanishi, T. Nagatomo, and S. Yoshida, “Analysis of MBE growth mode for GaN epilayers by RHEED,” J. Cryst. Growth 189–190, 364–369 (1998).
[Crossref]

Cho, Y.

T. Q. P. Vuong, G. Cassabois, P. Valvin, E. Rousseau, A. Summerfield, C. J. Mellor, Y. Cho, T. S. Cheng, J. D. Albar, L. Eaves, C. T. Foxon, P. H. Beton, S. V. Novikov, and B. Gil, “Deep ultraviolet emission in hexagonal boron nitride grown by high-temperature molecular beam epitaxy,” 2D Mater. 4(2), 021023 (2017).
[Crossref]

Cho, Y.-J.

Y.-J. Cho, A. Summerfield, A. Davies, T. S. Cheng, E. F. Smith, C. J. Mellor, A. N. Khlobystov, C. T. Foxon, L. Eaves, P. H. Beton, and S. V. Novikov, “Hexagonal Boron Nitride Tunnel Barriers Grown on Graphite by High Temperature Molecular Beam Epitaxy,” Sci. Rep. 6(1), 34474 (2016).
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J. Meng, X. Zhang, Y. Wang, Z. Yin, H. Liu, J. Xia, H. Wang, J. You, P. Jin, D. Wang, and X.-M. Meng, “Aligned Growth of Millimeter-Size Hexagonal Boron Nitride Single-Crystal Domains on Epitaxial Nickel Thin Film,” Small 13(18), 1604179 (2017).
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Figures (5)

Fig. 1
Fig. 1 (a)-(c) Snapshots of RHEED patterns during the growth of h-BN at 500 °C (Sample A), 1200 °C (Sample B) and 1300 °C (Sample C), respectively. The RHEED pattern transitions from polycrystalline rings to continuous streaks with samples growing at higher temperature. (d)-(f) SEM images of the same three sample surfaces.
Fig. 2
Fig. 2 XPS high-resolution spectrum of B 1s (a) and N 1s (b) for the h-BN Sample C. Micro-Raman spectrum of: (c) Sample A (in solid blue) as compared to the bare Ni substrate (in dotted black). The h-BN sample shows peaks at ~1365 and 1600 cm−1, corresponding to theoretical frequencies of 1394 (Raman-active; E2g) and 1627 cm−1 (IR-active LO mode; E1u); (d) Sample C, showing a strong and narrow Raman peak at 1360 cm−1 (FWHM of 13 cm−1). A secondary weak peak at 800 cm−1 is also present. Symmetry-breaking at the surface could turn the theoretically calculated mode at 747 (IR-active; A2u) or 818 cm−1 (IR- and Raman-forbidden; B1g) into a Raman-active mode.
Fig. 3
Fig. 3 Room-temperature PL spectra of three h-BN Samples A (in blue), B (in green) and C (in red). As growth temperature is increased, the short-wavelength emission is enhanced, and the longer-wavelength defect emissions are suppressed. The inset shows the PL spectrum measured at cryogenic temperature of Sample C.
Fig. 4
Fig. 4 Schematic band structure of BN near the band extrema. Although the bandgap is indirect, the phonon-assisted matrix element S is similarly strong to direct optical transition, and hence BN luminesces as a direct-gap material.
Fig. 5
Fig. 5 (a) Room-temperature PL emission of Sample C (in red) as compared to a commercial AlN epilayer template on sapphire (in black). (b) Integrated PL intensity of both samples measured at various laser excitation powers.

Equations (1)

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S 2 = p VBM 2 g 2 (ΔE+ ω phonon ) 2

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