First-Principles Predictions of Out-of-Plane Group IV and V Dimers as High-Symmetry, High-Spin Defects in Hexagonal Boron Nitride
Abstract
Hexagonal boron nitride (h-BN) has been recently found to host a variety of quantum point defects, which are promising candidates as single-photon sources for solid-state quantum nanophotonic applications. Most recently, optically addressable spin qubits in h-BN have been the focus of intensive research due to their unique potential in quantum computation, communication, and sensing. However, the number of high-symmetry, high-spin defects that are desirable for developing spin qubits in h-BN is highly limited. Here, we combine density functional theory (DFT) and quantum embedding theories to show that out-of-plane XNYi dimer defects (X, Y = C, N, P, and Si) form a new class of stable C3v spin-triplet defects in h-BN. We find that the dimer defects have a robust 3A2 ground state and 3E excited state, both of which are isolated from the h-BN bulk states. We show that 1E and 1A shelving states exist and they are positioned between the 3E and 3A2 states for all the dimer defects considered in this study. To support future experimental identification of the XNYi dimer defects, we provide extensive characterization of the defects in terms of their spin and optical properties. We predict that the zero-phonon line of the spin-triplet XNYi defectsmore »
- Authors:
-
[2];
[3];
[1]
- Ajou University (South Korea)
- Univ. of Chicago, IL (United States)
- Univ. of Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- National Research Foundation of Korea (NRF); Air Force Research Laboratory (AFRL), Air Force Office of Scientific Research (AFOSR)
- OSTI Identifier:
- 1845431
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 13; Journal Issue: 38; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; hexagonal boron nitride; spin defects; density functional theory; quantum embedding theory; solid-state quantum information; quantum nanophotonics; nitrides; oligomers; carbon; quantum mechanics; defects
Citation Formats
Bhang, Jooyong, Ma, He, Yim, Donggyu, Galli, Giulia, and Seo, Hosung. First-Principles Predictions of Out-of-Plane Group IV and V Dimers as High-Symmetry, High-Spin Defects in Hexagonal Boron Nitride. United States: N. p., 2021.
Web. doi:10.1021/acsami.1c16988.
Bhang, Jooyong, Ma, He, Yim, Donggyu, Galli, Giulia, & Seo, Hosung. First-Principles Predictions of Out-of-Plane Group IV and V Dimers as High-Symmetry, High-Spin Defects in Hexagonal Boron Nitride. United States. https://doi.org/10.1021/acsami.1c16988
Bhang, Jooyong, Ma, He, Yim, Donggyu, Galli, Giulia, and Seo, Hosung. Mon .
"First-Principles Predictions of Out-of-Plane Group IV and V Dimers as High-Symmetry, High-Spin Defects in Hexagonal Boron Nitride". United States. https://doi.org/10.1021/acsami.1c16988. https://www.osti.gov/servlets/purl/1845431.
@article{osti_1845431,
title = {First-Principles Predictions of Out-of-Plane Group IV and V Dimers as High-Symmetry, High-Spin Defects in Hexagonal Boron Nitride},
author = {Bhang, Jooyong and Ma, He and Yim, Donggyu and Galli, Giulia and Seo, Hosung},
abstractNote = {Hexagonal boron nitride (h-BN) has been recently found to host a variety of quantum point defects, which are promising candidates as single-photon sources for solid-state quantum nanophotonic applications. Most recently, optically addressable spin qubits in h-BN have been the focus of intensive research due to their unique potential in quantum computation, communication, and sensing. However, the number of high-symmetry, high-spin defects that are desirable for developing spin qubits in h-BN is highly limited. Here, we combine density functional theory (DFT) and quantum embedding theories to show that out-of-plane XNYi dimer defects (X, Y = C, N, P, and Si) form a new class of stable C3v spin-triplet defects in h-BN. We find that the dimer defects have a robust 3A2 ground state and 3E excited state, both of which are isolated from the h-BN bulk states. We show that 1E and 1A shelving states exist and they are positioned between the 3E and 3A2 states for all the dimer defects considered in this study. To support future experimental identification of the XNYi dimer defects, we provide extensive characterization of the defects in terms of their spin and optical properties. We predict that the zero-phonon line of the spin-triplet XNYi defects lies in the visible range (800 nm to 500 nm). We compute the zero-field splitting of the dimers’ spin to range from 1.79 GHz (SiNPio) to 29.5 GHz (CNNio). Furthermore, our results broaden the scope of high-spin defect candidates that would be useful for the development of spin-based solid-state quantum technologies in two-dimensional hexagonal boron nitride.},
doi = {10.1021/acsami.1c16988},
journal = {ACS Applied Materials and Interfaces},
number = 38,
volume = 13,
place = {United States},
year = {Mon Sep 20 00:00:00 EDT 2021},
month = {Mon Sep 20 00:00:00 EDT 2021}
}
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