TY - JOUR
T1 - Defect Engineering of Monoisotopic Hexagonal Boron Nitride Crystals via Neutron Transmutation Doping
AU - Li, Jiahan
AU - Glaser, Evan R.
AU - Elias, Christine
AU - Ye, Gaihua
AU - Evans, Dylan
AU - Xue, Lianjie
AU - Liu, Song
AU - Cassabois, Guillaume
AU - Gil, Bernard
AU - Valvin, Pierre
AU - Pelini, Thomas
AU - Yeats, Andrew L.
AU - He, Rui
AU - Liu, Bin
AU - Edgar, James H.
N1 - Funding Information:
This work was supported by the U.S. Department of Energy, Office of Nuclear Energy under DOE Idaho Operations Office Contract DE-AC07-051D14517 as part of a Nuclear Science User Facilities experiment. The crystal growth (J.L. and J.H.E.) in this study was supported by the Materials Engineering and Processing program of the National Science Foundation, award number CMMI 1538127. B.L. is grateful for the support by NSF grant CHE-1726332. The work performed at NRL (E.R.G. and A.L.Y.) was supported by the Office of Naval Research, and we thank Cory Cress (NRL) for helpful discussions. We would like to acknowledge the support of The Ohio State University Nuclear Reactor Laboratory and the assistance of Susan M. White, Lei Raymond Cao, Andrew Kauffman, and Kevin Herminghuysen for the irradiation services provided. Work at Texas Tech University (G.Y. and R.H.) was supported by an NSF CAREER grant (no. DMR-1760668). This work was financially supported in France by the contract BONASPES (ANR-19-CE30-0007-02) under the umbrella of the publicly funded Investissements d’Avenir program managed by the French ANR agency.
Publisher Copyright:
©
PY - 2021/12/14
Y1 - 2021/12/14
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85119927781&partnerID=8YFLogxK
U2 - 10.1021/acs.chemmater.1c02849
DO - 10.1021/acs.chemmater.1c02849
M3 - Article
AN - SCOPUS:85119927781
VL - 33
SP - 9231
EP - 9239
JO - Chemistry of Materials
JF - Chemistry of Materials
SN - 0897-4756
IS - 23
ER -