James Edgar

Spin defects in hexagonal boron nitride (hBN) are promising quantum systems for the design of flexible two-dimensional quantum sensing platforms. Here we rely on hBN crystals isotopically enriched with either 10B or 11B to investigate the isotope-dependent properties of a spin defect featuring a broadband photoluminescence signal in the near infrared. By analyzing the hyperfine structure of the spin defect while changing the boron isotope, we first confirm that it corresponds to the negatively charged boron-vacancy center (V B-). We then show that its spin coherence properties are slightly improved in 10B-enriched samples. This is supported by numerical simulations employing cluster correlation expansion methods, which reveal the importance of the hyperfine Fermi contact term for calculating the coherence time of point defects in hBN. Using cross-relaxation spectroscopy, we finally identify dark electron spin impurities as an additional source of decoherence. This work provides new insights into the properties of VB- spin defects, which are valuable for the future development of hBN-based quantum sensing foils.

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) 10B and 11B-enriched hBN crystalline flakes and a pyrolytic BN (pBN) reference sample. In h10BN 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.