First-Principles Predictions of Out-of-Plane Group IV and V Dimers as High-Symmetry, High-Spin Defects in Hexagonal Boron Nitride

Bhang, Jooyong; Ma, He; Yim, Donggyu; Galli, Giulia; Seo, Hosung

doi:10.1021/acsami.1c16988

Title: First-Principles Predictions of Out-of-Plane Group IV and V Dimers as High-Symmetry, High-Spin Defects in Hexagonal Boron Nitride

Journal Article · Mon Sep 20 00:00:00 EDT 2021 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.1c16988· OSTI ID:1845431

Bhang, Jooyong ^[1];

^[2]; Yim, Donggyu ^[1];

^[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)

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 X_NY_i dimer defects (X, Y = C, N, P, and Si) form a new class of stable C_3v 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 X_NY_i 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 X_NY_i 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 (Si_NP_i^o) to 29.5 GHz (C_NN_i^o). 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.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Research Foundation of Korea (NRF); Air Force Research Laboratory (AFRL), Air Force Office of Scientific Research (AFOSR)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1845431

Journal Information:: ACS Applied Materials and Interfaces, Vol. 13, Issue 38; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: First-Principles Predictions of Out-of-Plane Group IV and V Dimers as High-Symmetry, High-Spin Defects in Hexagonal Boron Nitride

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