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Tuning colour centres at a twisted hexagonal boron nitride interface

Nature Materials volume 21, pages 896–902 (2022)Cite this article

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Abstract

The colour centre platform holds promise for quantum technologies, and hexagonal boron nitride has attracted attention due to the high brightness and stability, optically addressable spin states and wide wavelength coverage discovered in its emitters. However, its application is hindered by the typically random defect distribution and complex mesoscopic environment. Here, employing cathodoluminescence, we demonstrate on-demand activation and control of colour centre emission at the twisted interface of two hexagonal boron nitride flakes. Further, we show that colour centre emission brightness can be enhanced by two orders of magnitude by tuning the twist angle. Additionally, by applying an external voltage, nearly 100% brightness modulation is achieved. Our ab initio GW and GW plus Bethe–Salpeter equation calculations suggest that the emission is correlated to nitrogen vacancies and that a twist-induced moiré potential facilitates electron–hole recombination. This mechanism is further exploited to draw nanoscale colour centre patterns using electron beams.

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Fig. 1: Defect emission from T-hBN interface.
Fig. 2: Angle-dependent brightness and crystal structures of T-hBN.
Fig. 3: Defect type assignment by GW-BSE calculation.
Fig. 4: Optical modulation of the emitter via external voltage.
Fig. 5: Trap-state saturation and electron-beam patterning.

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All data are available in the main text or the Supplementary Information.

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Acknowledgements

This work was supported primarily by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division under contract no. DE-AC02-05-CH11231, within the sp2-Bonded Materials Program (KC2207), which provided for the development of the project concept and theoretical calculations. CL and HRTEM measurements were provided by The Molecular Foundry, supported under the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division under contract no. DE-AC02-05-CH11231. Additional support was provided by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division under contract no. DE-AC02-05-CH11231, within the van der Waals Bonded Materials Program (KCWF16), which provided for sample fabrication, and within the Theory of Materials Program, which provided theoretical methods and analyses. Preparation of the TEM grid suspended samples was provided by the National Science Foundation under grant DMR-1807322. C.S. gratefully acknowledges the financial support of a Kavli Energy NanoScience Institute Heising-Simons Postdoctoral Fellowship. K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan (grant no. JPMXP0112101001) and the Japan Society for the Promotion of Science KAKENHI (grant nos 19H05790 and JP20H00354). W.Z. and F.Z. acknowledge the support from the Guangdong Innovation Research Team Project (no. 2017ZT07C062), Guangdong Provincial Key-Lab programme (no. 2019B030301001), Shenzhen Municipal Key-Lab programme (ZDSYS20190902092905285) and Centre for Computational Science and Engineering at Southern University of Science and Technology. J.-H.P. and J.K. acknowledge the support from the US Army Research Office Multidisciplinary University Research Initiative under grant no. W911NF-18-1-0431 and the US Army Research Office through the Institute for Soldier Nanotechnologies at MIT, under cooperative agreement no. W911NF-18-2-0048.

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Author notes

  1. These authors contributed equally: Cong Su, Fang Zhang, Salman Kahn.

Authors and Affiliations

  1. Department of Physics, University of California, Berkeley, CA, USA

    Cong Su, Fang Zhang, Salman Kahn, Brian Shevitski, Jingwei Jiang, Chunhui Dai, Alex Ungar, Feng Wang, Michael Crommie, Steven G. Louie & Alex Zettl

  2. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Cong Su, Fang Zhang, Salman Kahn, Brian Shevitski, Jingwei Jiang, Chunhui Dai, Alex Ungar, Feng Wang, Michael Crommie, Steven G. Louie & Alex Zettl

  3. Kavli Energy NanoSciences Institute at the University of California, Berkeley, CA, USA

    Cong Su, Brian Shevitski, Chunhui Dai, Alex Ungar, Feng Wang, Michael Crommie & Alex Zettl

  4. Department of Physics, Southern University of Science and Technology, Shenzhen, China

    Fang Zhang & Wenqing Zhang

  5. Institute of Applied Physics and Materials Engineering, University of Macau, Macau, China

    Fang Zhang & Zikang Tang

  6. The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Brian Shevitski & Shaul Aloni

  7. Electrical Engineering and Computer Sciences, Massachusetts Institute of Technology, Cambridge, MA, USA

    Ji-Hoon Park & Jing Kong

  8. Research Centre for Functional Materials, National Institute for Materials Science, Tsukuba, Japan

    Kenji Watanabe

  9. International Centre for Materials Nanoarchitectonics, National Institute for Materials Science, Tsukuba, Japan

    Takashi Taniguchi

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Contributions

C.S., A.Z. and S.A. conceived the experiments. A.Z. supervised the whole project. S.G.L. supervised the theoretical studies. C.S. and S.A. designed and performed the regular, in situ and cryo-CL and HRTEM experiments. F.Z. performed the calculations and, with J.J. and S.G.L., performed the theory analyses. S.K. prepared the samples and fabricated the devices. C.D. and A.U. aided in sample preparations. J.-H.P. and J.K. prepared the monolayer hBN samples. K.W. and T.T. provided the bulk hBN samples. C.S. wrote the paper. All the authors were involved in the paper revisions.

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Correspondence to Steven G. Louie, Shaul Aloni or Alex Zettl.

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Nature Materials thanks Sajid Ali and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–13, Table 1 and Discussion.

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Su, C., Zhang, F., Kahn, S. et al. Tuning colour centres at a twisted hexagonal boron nitride interface. Nat. Mater. 21, 896–902 (2022). https://doi.org/10.1038/s41563-022-01303-4

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