4.8 Article

Defect Engineering of Monoisotopic Hexagonal Boron Nitride Crystals via Neutron Transmutation Doping

期刊

CHEMISTRY OF MATERIALS
卷 33, 期 23, 页码 9231-9239

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AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.1c02849

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资金

  1. U.S. Department of Energy, Office of Nuclear Energy under DOE Idaho Operations Office [DE-AC07-051D14517]
  2. Materials Engineering and Processing program of the National Science Foundation [CMMI 1538127]
  3. NSF [CHE-1726332]
  4. Office of Naval Research
  5. Ohio State University Nuclear Reactor Laboratory
  6. NSF CAREER [DMR1760668]
  7. BONASPES [ANR-19-CE30-0007-02]

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This study investigates the impact of neutron irradiation on single-isotope boron nitride crystal flakes, revealing new Raman bands associated with B-related vacancies or defects, as well as identifying a high-spin defect center due to negatively charged boron vacancies. High-temperature annealing partially restores the vibrational and optical properties of boron nitride, offering insights for defect-engineered applications such as quantum information and sensing.
The nature of point defects in hexagonal boron nitride (hBN) is of current interest for the potential to alter its optical and electrical properties. The strong interaction between neutrons and the boron-10 isotope makes neutron irradiation a controllable way to introduce point defects in hBN. In this study, we perform Raman spectroscopy, photoluminescence, electron paramagnetic resonance (EPR), and optically detected magnetic resonance (ODMR) characterization of neutron-irradiated monoisotopic (hBN with a single boron isotope) B-10- and B-11-enriched hBN crystalline flakes and a pyrolytic BN (pBN) reference sample. In h(10)BN and pBN, neutron irradiation produced two new Raman bands at 450 and 1335 cm(-1), which could be associated with B-related vacancies or defects. The near-bandedge optical emission was also significantly impacted by the neutron irradiation. EPR measurements clarified the origin of a high-spin defect center due to negatively charged boron vacancies, which was recently reported for similar neutron-irradiated hBN crystals. The ODMR experiments further confirmed this assignment. High-temperature annealing partially recovered some of the hBN vibrational and optical properties. Our results are helpful to identify the nature of defects in hBN and enable defect-engineered applications such as quantum information and sensing.

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