Homoepitaxial growth of isotopically enriched h10BN layers on h11BN crystals by high-temperature molecular beam epitaxy
Source abstract
Abstract
Abstract Isotope-enriched bulk hexagonal boron nitride (hBN) crystals have enhanced properties that improve the performance of nanophotonic and quantum technologies. Developing methods to deposit epitaxial layers on such crystals enables the exciting prospects of producing isotope-engineered hBN layers and heterostructures. Here, we demonstrate the homoepitaxial growth of hBN with phase-separated 10 B and 11 B isotopes by high-temperature molecular beam epitaxy (HT-MBE). Controlled nucleation, improved surface uniformity, and step-flow growth of an h 10 BN epilayer were achieved by etching the h 11 BN bulk crystals with molecular hydrogen. The alignment of the h 10 BN epilayer and host h 11 BN lattices was confirmed by lattice-resolved atomic force microscopy. Micro-Raman spectroscopy and scattering-type scanning near-field optical microscopy show that the bulk h 11 BN and h 10 BN epilayer have distinct phonon energies, with no intermixing of the van der Waals layers, thus enabling the different boron isotopes to be spatially separated in the heterostructure. This work demonstrates the potential of HT-MBE to produce isotopic heterostructures of hBN to advance future nanophotonic and quantum technologies.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: Graphene research and applications · Boron and Carbon Nanomaterials Research · 2D Materials and Applications
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (57)
Show source-provided references
1. Vuong, T. Q. P. et al. Deep ultraviolet emission in hexagonal boron nitride grown by high-temperature molecular beam epitaxy. 2D Mater. 4, 021023 (2017).10.1088/2053-1583/aa604a ↗
2. Elias, C. et al. Direct band-gap crossover in epitaxial monolayer boron nitride. Nat. Commun. 10, 2639 (2019).10.1038/s41467-019-10610-5 ↗
3. Rousseau, A. et al. Spatially-resolved UV-C emission in epitaxial monolayer boron nitride. 2D Mater. 11, 025026 (2024).10.1088/2053-1583/ad2f45 ↗
4. Tran, T. T., Bray, K., Ford, M. J., Toth, M. & Aharonovich, I. Quantum emission from hexagonal boron nitride monolayers. Nat. Nano 11, 37–41 (2016).10.1038/nnano.2015.242 ↗
5. Aharonovich, I., Tetienne, J.-P. & Toth, M. Quantum emitters in hexagonal boron nitride. Nano Lett. 22, 9227–9235 (2022).10.1021/acs.nanolett.2c03743 ↗
6. Mendelson, N. et al. Identifying carbon as the source of visible single-photon emission from hexagonal boron nitride. Nat. Mater. 20, 321–328 (2021).10.1038/s41563-020-00850-y ↗
7. Stern, H. L. et al. A quantum coherent spin in hexagonal boron nitride at ambient conditions. Nat. Mater. 23, 1379–1385 (2024).10.1038/s41563-024-01887-z ↗
8. Stern, H. L. et al. Room-temperature optically detected magnetic resonance of single defects in hexagonal boron nitride. Nat. Commun. 13, 618 (2022).10.1038/s41467-022-28169-z ↗
9. Gao, X. et al. Nuclear spin polarization and control in hexagonal boron nitride. Nat. Mater. 21(9 21), 1024–1028 (2022).10.1038/s41563-022-01329-8 ↗
10. Rousseau, A. et al. Bernal Boron nitride crystals identified by deep-ultraviolet Cryomicroscopy. ACS Nano 16, 2756–2761 (2022).10.1021/acsnano.1c09717 ↗
11. Iwański, J. et al. Revealing polytypism in 2D boron nitride with UV photoluminescence. NPJ 2D Mater. Appl. 8, 72 (2024).10.1038/s41699-024-00511-7 ↗
12. Moon, S. et al. Wafer-scale AA-stacked hexagonal boron nitride grown on a GaN substrate. Nat. Mater. 24, 843–851 (2025).10.1038/s41563-025-02173-2 ↗
13. Rousseau, A. et al. Determination of the optical bandgap of the Bernal and rhombohedral boron nitride polymorphs. Phys. Rev. Mater. 5, 064602 (2021).10.1103/PhysRevMaterials.5.064602 ↗
14. Yasuda, K., Wang, X., Watanabe, K., Taniguchi, T. & Jarillo-Herrero, P. Stacking-engineered ferroelectricity in bilayer boron nitride. Science 372, 1458–1462 (2021).10.1126/science.abd3230 ↗
15. Lv, M. et al. Spatially resolved polarization manipulation of ferroelectricity in twisted hBN. Adv. Mater. 34, 2203990 (2022).10.1002/adma.202203990 ↗
16. Vizner Stern, M. et al. Interfacial ferroelectricity by van der Waals sliding. Science 372, 1462–1466 (2021).10.1126/science.abe8177 ↗
17. Wong, S. et al. Epitaxial ferroelectric hexagonal boron nitride grown on graphene. Adv. Mater. 37, 2414442 (2025).10.1002/adma.202414442 ↗
18. Alemoush, Z. et al. Status of h-BN quasi-bulk crystals and high efficiency neutron detectors. J. Appl. Phys. 135, 175704 (2024).10.1063/5.0179610 ↗
19. Li, J., Tingsuwatit, A., Alemoush, Z., Lin, J. Y. & Jiang, H. X. Ultrawide bandgap semiconductor h-BN for direct detection of fast neutrons. APL Mater. 13, 11101 (2025).10.1063/5.0232896 ↗
20. Janzen, E. et al. Boron and nitrogen isotope effects on hexagonal boron nitride properties. Adv. Mater. 36, 2306033 (2024).10.1002/adma.202306033 ↗
21. Vuong, T. Q. P. et al. Isotope engineering of van der Waals interactions in hexagonal boron nitride. Nat. Mater. 17, 152–158 (2018).10.1038/nmat5048 ↗
22. Mercado, E. et al. Isotopically enhanced thermal conductivity in few-layer hexagonal boron nitride: implications for thermal management. ACS Appl Nano Mater. 3, 12148–12156 (2020).10.1021/acsanm.0c02647 ↗
23. Yuan, C. et al. Modulating the thermal conductivity in hexagonal boron nitride via controlled boron isotope concentration. Commun. Phys. 2, 43 (2019).10.1038/s42005-019-0145-5 ↗
24. Cai, Q. et al. Outstanding thermal conductivity of single atomic layer isotope-modified boron nitride. Phys. Rev. Lett. 125, 085902 (2020).10.1103/PhysRevLett.125.085902 ↗
25. Chen, M. et al. Van der Waals isotope heterostructures for engineering phonon polariton dispersions. Nat. Commun. 14, 4782 (2023).10.1038/s41467-023-40449-w ↗
26. Giles, A. J. et al. Ultralow-loss polaritons in isotopically pure boron nitride. Nat. Mater. 17, 134–139 (2018).10.1038/nmat5047 ↗
27. Dai, S. et al. Tunable phonon polaritons in atomically thin van der Waals crystals of boron nitride. Science 343, 1125–1129 (2014).10.1126/science.1246833 ↗
28. Gong, R. et al. Isotope engineering for spin defects in van der Waals materials. Nat. Commun. 15, 104 (2024).10.1038/s41467-023-44494-3 ↗
29. Haykal, A. et al. Decoherence of VB- spin defects in monoisotopic hexagonal boron nitride. Nat. Commun. 13, 4347 (2022).10.1038/s41467-022-31743-0 ↗
30. Liu, S. et al. Single crystal growth of millimeter-sized monoisotopic hexagonal boron nitride. Chem. Mater. 30, 6222–6225 (2018).10.1021/acs.chemmater.8b02589 ↗
31. Li, J. et al. Single crystal growth of monoisotopic hexagonal boron nitride from a Fe–Cr flux. J. Mater. Chem. C. Mater. 8, 9931–9935 (2020).10.1039/D0TC02143A ↗
32. Sutter, P., Lahiri, J., Albrecht, P. & Sutter, E. Chemical vapor deposition and etching of high-quality monolayer hexagonal boron nitride films. ACS Nano 5, 7303–7309 (2011).10.1021/nn202141k ↗
33. Ma, K. Y. et al. Epitaxial single-crystal hexagonal boron nitride multilayers on Ni (111). Nature 606, 88–93 (2022).10.1038/s41586-022-04745-7 ↗
34. Wang, G. et al. Wafer-scale single crystal hexagonal boron nitride layers grown by submicron-spacing vapor deposition. Small 19, 2301086 (2023).10.1002/smll.202301086 ↗
35. Wang, L. et al. Epitaxial growth of a 100-square-centimetre single-crystal hexagonal boron nitride monolayer on copper. Nature 570, 91–95 (2019).10.1038/s41586-019-1226-z ↗
36. Wang, L. et al. Growth and etching of monolayer hexagonal boron nitride. Adv. Mater. 27, 4858–4864 (2015).10.1002/adma.201501166 ↗
37. Bansal, A. et al. Substrate modification during chemical vapor deposition of hBN on sapphire. ACS Appl. Mater. Interfaces 13, 54516–54526 (2021).10.1021/acsami.1c14591 ↗
38. Kim, J. et al. Conformal growth of hexagonal boron nitride on high-aspect-ratio silicon-based nanotrenches. Chem. Mater. 35, 2429–2438 (2023).10.1021/acs.chemmater.2c03568 ↗
39. Summerfield, A. et al. Moiré-modulated conductance of hexagonal boron nitride tunnel barriers. Nano Lett. 18, 4241–4246 (2018).10.1021/acs.nanolett.8b01223 ↗
40. Pierucci, D. et al. Van der Waals epitaxy of two-dimensional single-layer h-BN on graphite by molecular beam epitaxy: Electronic properties and band structure. Appl Phys. Lett. 112, 253102 (2018).10.1063/1.5029220 ↗
41. Cheng, T. S. et al. High-temperature molecular beam epitaxy of hexagonal boron nitride layers. J. Vac. Sci. Technol. B Nanotechnol. Microelectron.: Mater. Process. Meas. Phenom. 36, 02D103 (2018).10.1116/1.5011280 ↗
42. Thomas, J. et al. Step-flow growth of graphene-boron nitride lateral heterostructures by molecular beam epitaxy. 2D Mater. 7, 035014 (2020).10.1088/2053-1583/ab89e7 ↗
43. Wrigley, J. et al. Epitaxy of boron nitride monolayers for graphene-based lateral heterostructures. 2D Mater. 8, 034001 (2021).10.1088/2053-1583/abea66 ↗
44. Binder, J. et al. Homoepitaxy of boron nitride on exfoliated hexagonal boron nitride flakes. Nano Lett. 24, 6990–6996 (2024).10.1021/acs.nanolett.4c01310 ↗
45. Jean-Remy, P. M., Cabral, M. J. & Davis, R. F. Chemical vapor deposition of sp2-boron nitride on mechanically polished pyrolytic boron nitride substrates. J. Vac. Sci. Technol. A 40, 42203 (2022).10.1116/6.0001784 ↗
46. Novikov, S. V. & Foxon, C. T. Unintentional boron incorporation in AlGaN layers grown by plasma-assisted MBE using highly efficient nitrogen RF plasma-sources. J. Cryst. Growth 477, 154–158 (2017).10.1016/j.jcrysgro.2017.01.007 ↗
47. Chen, L. et al. Direct observation of layer-stacking and oriented wrinkles in multilayer hexagonal boron nitride. 2D Mater. 8, 024001 (2021).10.1088/2053-1583/abd41e ↗
48. Stehle, Y. Y. et al. Anisotropic etching of hexagonal boron nitride and graphene: question of edge terminations. Nano Lett. 17, 7306–7314 (2017).10.1021/acs.nanolett.7b02841 ↗
49. Liu, H. et al. Structure evolution of hBN grown on molten Cu by regulating precursor flux during chemical vapor deposition. 2D Mater. 9, 015004 (2021).10.1088/2053-1583/ac2e59 ↗
50. Stehle, Y. et al. Synthesis of hexagonal boron nitride monolayer: control of nucleation and crystal morphology. Chem. Mater. 27, 8041–8047 (2015).10.1021/acs.chemmater.5b03607 ↗
51. Zhang, L. & Ding, F. The stable interfaces between various edges of hBN and step edges of Cu surface in hBN epitaxial growth: a comprehensive theoretical exploration. 2D Mater. 8, 034004 (2021).10.1088/2053-1583/abf80f ↗
52. Falin, A. et al. Anomalous isotope effect on the mechanical properties of a single atomic layer of Boron Nitride. Nat. Commun. 14, 1–9 (2023).10.1038/s41467-023-41148-2 ↗
53. Chiodini, S. et al. Moiré modulation of Van der Waals potential in twisted hexagonal boron nitride. ACS Nano 16, (2021).10.1021/acsnano.1c11107 ↗
54. Mohammad, A. et al. Effective substrate for the growth of multilayer h-BN on sapphire—substrate off-cut, pre-growth, and post-growth conditions in metal-organic vapor phase epitaxy. 2D Mater. 10, 025010 (2023).10.1088/2053-1583/acb44a ↗
55. Bradford, J. et al. Graphene nanoribbons with hBN passivated edges grown by high-temperature molecular beam epitaxy. 2D Mater. 10, 035035 (2023).10.1088/2053-1583/acdefc ↗
56. Hutchins, W. et al. Ultrafast evanescent heat transfer across solid interfaces via hyperbolic phonon–polariton modes in hexagonal boron nitride. Nat. Mater. 24, 698–706 (2025).10.1038/s41563-025-02154-5 ↗
57. Brasington, A. et al. Phonon lifetimes in boron-isotope-enriched graphene-hexagonal boron nitride devices. Phys. Status Solidi (RRL) – Rapid Res. Lett. 16, 2200030 (2022).10.1002/pssr.202200030 ↗