Intersystem crossing and exciton–defect coupling of spin defects in hexagonal boron nitride
Abstract
Despite the recognition of two-dimensional (2D) systems as emerging and scalable host materials of single-photon emitters or spin qubits, the uncontrolled, and undetermined chemical nature of these quantum defects has been a roadblock to further development. Leveraging the design of extrinsic defects can circumvent these persistent issues and provide an ultimate solution. Here, we established a complete theoretical framework to accurately and systematically design quantum defects in wide-bandgap 2D systems. With this approach, essential static and dynamical properties are equally considered for spin qubit discovery. In particular, many-body interactions such as defect–exciton couplings are vital for describing excited state properties of defects in ultrathin 2D systems. Meanwhile, nonradiative processes such as phonon-assisted decay and intersystem crossing rates require careful evaluation, which competes together with radiative processes. From a thorough screening of defects based on first-principles calculations, we identify promising single-photon emitters such as SiVV and spin qubits such as TiVV and MoVV in hexagonal boron nitride. This work provided a complete first-principles theoretical framework for defect design in 2D materials.
- Authors:
-
- University of California, Santa Cruz, CA (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- University of California, Santa Cruz, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC); National Science Foundation (NSF); USDOE Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1888623
- Report Number(s):
- LLNL-JRNL-820110
Journal ID: ISSN 2057-3960; 1031303; TRN: US2309909
- Grant/Contract Number:
- AC52-07NA27344; DMR-1760260; DMR-1956015; DMR-1747426; SC0012704; AST 1828315; AC02-05CH11231; ACI-1548562
- Resource Type:
- Accepted Manuscript
- Journal Name:
- npj Computational Materials
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2057-3960
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; computational methods; electronic structure; electronics; photonics; device physics; spintronics
Citation Formats
Smart, Tyler J., Li, Kejun, Xu, Junqing, and Ping, Yuan. Intersystem crossing and exciton–defect coupling of spin defects in hexagonal boron nitride. United States: N. p., 2021.
Web. doi:10.1038/s41524-021-00525-5.
Smart, Tyler J., Li, Kejun, Xu, Junqing, & Ping, Yuan. Intersystem crossing and exciton–defect coupling of spin defects in hexagonal boron nitride. United States. https://doi.org/10.1038/s41524-021-00525-5
Smart, Tyler J., Li, Kejun, Xu, Junqing, and Ping, Yuan. Fri .
"Intersystem crossing and exciton–defect coupling of spin defects in hexagonal boron nitride". United States. https://doi.org/10.1038/s41524-021-00525-5. https://www.osti.gov/servlets/purl/1888623.
@article{osti_1888623,
title = {Intersystem crossing and exciton–defect coupling of spin defects in hexagonal boron nitride},
author = {Smart, Tyler J. and Li, Kejun and Xu, Junqing and Ping, Yuan},
abstractNote = {Despite the recognition of two-dimensional (2D) systems as emerging and scalable host materials of single-photon emitters or spin qubits, the uncontrolled, and undetermined chemical nature of these quantum defects has been a roadblock to further development. Leveraging the design of extrinsic defects can circumvent these persistent issues and provide an ultimate solution. Here, we established a complete theoretical framework to accurately and systematically design quantum defects in wide-bandgap 2D systems. With this approach, essential static and dynamical properties are equally considered for spin qubit discovery. In particular, many-body interactions such as defect–exciton couplings are vital for describing excited state properties of defects in ultrathin 2D systems. Meanwhile, nonradiative processes such as phonon-assisted decay and intersystem crossing rates require careful evaluation, which competes together with radiative processes. From a thorough screening of defects based on first-principles calculations, we identify promising single-photon emitters such as SiVV and spin qubits such as TiVV and MoVV in hexagonal boron nitride. This work provided a complete first-principles theoretical framework for defect design in 2D materials.},
doi = {10.1038/s41524-021-00525-5},
journal = {npj Computational Materials},
number = 1,
volume = 7,
place = {United States},
year = {Fri Apr 30 00:00:00 EDT 2021},
month = {Fri Apr 30 00:00:00 EDT 2021}
}
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