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Site-Specific Fabrication of Blue Quantum Emitters in Hexagonal Boron Nitride

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Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Photonics 2022, 9, 6, 2170-2177
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    Site-Specific Fabrication of Blue Quantum Emitters in Hexagonal Boron Nitride
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    • Angus Gale
      Angus Gale
      School of Mathematical and Physical Sciences, University of Technology Sydney, Ultimo, Sydney, New South Wales 2007, Australia
      More by Angus Gale
    • Chi Li
      Chi Li
      School of Mathematical and Physical Sciences, University of Technology Sydney, Ultimo, Sydney, New South Wales 2007, Australia
      More by Chi Li
      Orcidhttps://orcid.org/0000-0002-8424-9721
    • Yongliang Chen
      Yongliang Chen
      School of Mathematical and Physical Sciences, University of Technology Sydney, Ultimo, Sydney, New South Wales 2007, Australia
      More by Yongliang Chen
    • Kenji Watanabe
      Kenji Watanabe
      Research Center for Functional Materials, National Institute for Materials Science, Tsukuba 305-0044, Japan
      More by Kenji Watanabe
      Orcidhttps://orcid.org/0000-0003-3701-8119
    • Takashi Taniguchi
      Takashi Taniguchi
      International Center for Materials Nanoarchitectonics, National Institute for Materials Science, Tsukuba 305-0044, Japan
      More by Takashi Taniguchi
      Orcidhttps://orcid.org/0000-0002-1467-3105
    • Igor Aharonovich
      Igor Aharonovich
      School of Mathematical and Physical Sciences, University of Technology Sydney, Ultimo, Sydney, New South Wales 2007, Australia
      ARC Centre of Excellence for Transformative Meta-Optical Systems, University of Technology Sydney, Ultimo, Sydney, New South Wales 2007, Australia
      More by Igor Aharonovich
      Orcidhttps://orcid.org/0000-0003-4304-3935
    • Milos Toth*
      Milos Toth
      School of Mathematical and Physical Sciences, University of Technology Sydney, Ultimo, Sydney, New South Wales 2007, Australia
      ARC Centre of Excellence for Transformative Meta-Optical Systems, University of Technology Sydney, Ultimo, Sydney, New South Wales 2007, Australia
      *Email: [email protected]
      More by Milos Toth
      Orcidhttps://orcid.org/0000-0003-1564-4899
    Other Access OptionsSupporting Information (1)

    ACS Photonics

    Cite this: ACS Photonics 2022, 9, 6, 2170–2177
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    https://doi.org/10.1021/acsphotonics.2c00631
    Published May 18, 2022
    Copyright © 2022 American Chemical Society
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    Abstract

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    Hexagonal boron nitride (hBN) is gaining considerable attention as a solid-state host of quantum emitters from the ultraviolet to the near-infrared spectral ranges. However, the atomic structures of most of the emitters are speculative or unknown, and emitter fabrication methods typically suffer from poor reproducibility, spatial accuracy, or spectral specificity. Here, we present a robust, electron beam technique for site-specific fabrication of blue quantum emitters with a zero-phonon line at 436 nm (2.8 eV). We show that the emission intensity is proportional to electron dose and that the efficacy of the fabrication method correlates with a defect emission at 305 nm (4.1 eV). We attribute blue emitter generation to the fragmentation of carbon clusters by electron impact and show that the robustness and universality of the emitter fabrication technique are enhanced by a pre-irradiation annealing treatment. Our results provide important insights into photophysical properties and structure of defects in hBN and a framework for site-specific fabrication of quantum emitters in hBN.

    Copyright © 2022 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsphotonics.2c00631.

    • Supporting Information file provides spectrometer calibration data, CL and PL autocorrelation data, and a PL saturation measurement (PDF)

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    Cited By

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    This article is cited by 20 publications.

    1. Jake Horder, Dominic Scognamiglio, Ádám Ganyecz, Viktor Ivády, Nathan Coste, Mehran Kianinia, Milos Toth, Igor Aharonovich. Near-Coherent Quantum Emitters in Hexagonal Boron Nitride with Discrete Polarization Axes. ACS Photonics 2024, Article ASAP.
    2. Marek Maciaszek, Lukas Razinkovas. Blue Quantum Emitter in Hexagonal Boron Nitride and a Carbon Chain Tetramer: a First-Principles Study. ACS Applied Nano Materials 2024, 7 (16) , 18979-18985. https://doi.org/10.1021/acsanm.4c02722
    3. Sakal Singla, Pragya Joshi, Gabriel I. López-Morales, Suman Sarkar, Suman Sarkar, Johannes Flick, Biswanath Chakraborty. Probing Correlation of Optical Emission and Defect Sites in Hexagonal Boron Nitride by High-Resolution STEM-EELS. Nano Letters 2024, 24 (30) , 9212-9220. https://doi.org/10.1021/acs.nanolett.4c01477
    4. Anand Kumar, Chanaprom Cholsuk, Mohammad N. Mishuk, Mouli Hazra, Clotilde Pillot, Tjorben Matthes, Tanveer A. Shaik, Aslı Çakan, Volker Deckert, Sujin Suwanna, Tobias Vogl. Comparative Study of Quantum Emitter Fabrication in Wide Bandgap Materials Using Localized Electron Irradiation. ACS Applied Optical Materials 2024, 2 (2) , 323-332. https://doi.org/10.1021/acsaom.3c00441
    5. Anand Kumar, Çağlar Samaner, Chanaprom Cholsuk, Tjorben Matthes, Serkan Paçal, Yağız Oyun, Ashkan Zand, Robert J. Chapman, Grégoire Saerens, Rachel Grange, Sujin Suwanna, Serkan Ateş, Tobias Vogl. Polarization Dynamics of Solid-State Quantum Emitters. ACS Nano 2024, 18 (7) , 5270-5281. https://doi.org/10.1021/acsnano.3c08940
    6. Fei Ren, Zongwei Xu, Yiyuan Wu, Xiaogang Wang, Yanling Guo, Lin Chen, Ying Song, Bing Dong. Color Centers in Hexagonal Boron Nitride Nanosheet-Based Heterojunctions: Implications for Quantum Emitters and Ultrathin Sensors. ACS Applied Nano Materials 2024, 7 (3) , 3436-3444. https://doi.org/10.1021/acsanm.3c06179
    7. Zhibo Dang, Yuxiang Chen, Zheyu Fang. Cathodoluminescence Nanoscopy: State of the Art and Beyond. ACS Nano 2023, 17 (24) , 24431-24448. https://doi.org/10.1021/acsnano.3c07593
    8. Lesley Spencer, Jake Horder, Sejeong Kim, Milos Toth, Igor Aharonovich. Monolithic Integration of Single Quantum Emitters in hBN Bullseye Cavities. ACS Photonics 2023, 10 (12) , 4417-4424. https://doi.org/10.1021/acsphotonics.3c01282
    9. Milad Nonahal, Jake Horder, Angus Gale, Lu Ding, Chi Li, Madeline Hennessey, Son Tung Ha, Milos Toth, Igor Aharonovich. Deterministic Fabrication of a Coupled Cavity–Emitter System in Hexagonal Boron Nitride. Nano Letters 2023, 23 (14) , 6645-6650. https://doi.org/10.1021/acs.nanolett.3c01836
    10. Angus Gale, Dominic Scognamiglio, Ivan Zhigulin, Benjamin Whitefield, Mehran Kianinia, Igor Aharonovich, Milos Toth. Manipulating the Charge State of Spin Defects in Hexagonal Boron Nitride. Nano Letters 2023, 23 (13) , 6141-6147. https://doi.org/10.1021/acs.nanolett.3c01678
    11. Hongbing Cai, Shihao Ru, Zhengzhi Jiang, John Jun Hong Eng, Ruihua He, Fu-li Li, Yansong Miao, Jesús Zúñiga-Pérez, Weibo Gao. Spin Defects in hBN assisted by Metallic Nanotrenches for Quantum Sensing. Nano Letters 2023, 23 (11) , 4991-4996. https://doi.org/10.1021/acs.nanolett.3c00849
    12. Sai Krishna Narayanan, Pratibha Dev. Substrate-Induced Modulation of Quantum Emitter Properties in 2D Hexagonal Boron Nitride: Implications for Defect-Based Single Photon Sources in 2D Layers. ACS Applied Nano Materials 2023, 6 (5) , 3446-3452. https://doi.org/10.1021/acsanm.2c05233
    13. K. Parto, S. I. Azzam, N. Lewis, S. D. Patel, S. Umezawa, K. Watanabe, T. Taniguchi, G. Moody. Cavity-Enhanced 2D Material Quantum Emitters Deterministically Integrated with Silicon Nitride Microresonators. Nano Letters 2022, 22 (23) , 9748-9756. https://doi.org/10.1021/acs.nanolett.2c03151
    14. Igor Aharonovich, Jean-Philippe Tetienne, Milos Toth. Quantum Emitters in Hexagonal Boron Nitride. Nano Letters 2022, 22 (23) , 9227-9235. https://doi.org/10.1021/acs.nanolett.2c03743
    15. Song Li, Adam Gali. Identification of an Oxygen Defect in Hexagonal Boron Nitride. The Journal of Physical Chemistry Letters 2022, 13 (41) , 9544-9551. https://doi.org/10.1021/acs.jpclett.2c02687
    16. Ivan Zhigulin, Karin Yamamura, Viktor Ivády, Angus Gale, Jake Horder, Charlene J Lobo, Mehran Kianinia, Milos Toth, Igor Aharonovich. Photophysics of blue quantum emitters in hexagonal boron nitride. Materials for Quantum Technology 2023, 3 (1) , 015002. https://doi.org/10.1088/2633-4356/acb87f
    17. Federica Bianco, Emilio Corte, Sviatoslav Ditalia Tchernij, Jacopo Forneris, Filippo Fabbri. Engineering Multicolor Radiative Centers in hBN Flakes by Varying the Electron Beam Irradiation Parameters. Nanomaterials 2023, 13 (4) , 739. https://doi.org/10.3390/nano13040739
    18. Jake Horder, Simon J.U. White, Angus Gale, Chi Li, Kenji Watanabe, Takashi Taniguchi, Mehran Kianinia, Igor Aharonovich, Milos Toth. Coherence Properties of Electron-Beam-Activated Emitters in Hexagonal Boron Nitride Under Resonant Excitation. Physical Review Applied 2022, 18 (6) https://doi.org/10.1103/PhysRevApplied.18.064021
    19. Sébastien Roux, Clarisse Fournier, Kenji Watanabe, Takashi Taniguchi, Jean-Pierre Hermier, Julien Barjon, Aymeric Delteil. Cathodoluminescence monitoring of quantum emitter activation in hexagonal boron nitride. Applied Physics Letters 2022, 121 (18) , 184002. https://doi.org/10.1063/5.0126357
    20. Rachael Klaiss, Joshua Ziegler, David Miller, Kara Zappitelli, Kenji Watanabe, Takashi Taniguchi, Benjamín Alemán. Uncovering the morphological effects of high-energy Ga + focused ion beam milling on hBN single-photon emitter fabrication. The Journal of Chemical Physics 2022, 157 (7) , 074703. https://doi.org/10.1063/5.0097581
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    ACS Photonics

    Cite this: ACS Photonics 2022, 9, 6, 2170–2177
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsphotonics.2c00631
    Published May 18, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

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