First-principles calculations of h-BN monolayers by doping with oxygen and sulfur

Zhang, Zhaofu; Zhou, Tiege; Zuo, Xu

doi:10.7498/aps.62.083102

Cited by 11 publications

(4 citation statements)

References 26 publications

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“…While much work has focused on the negatively charged nitrogen vacancy center (N V -1 ) in diamond, [5][6] hexagonal boron nitride (h-BN) also has the potential to host many such color centres. [7][8][9][10][11][12][13][14] Defect occurrences are not only naturally occurring [15][16] but can also be artificially induced and controlled, 17 leading to device possibilities.…”

Section: Introductionmentioning

confidence: 99%

Understanding and Calibrating Density-Functional-Theory Calculations Describing the Energy and Spectroscopy of Defect Sites in Hexagonal Boron Nitride

Reimers

Ali

Kobayashi

et al. 2018

J. Chem. Theory Comput.

145

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Defect states in 2D materials present many possible uses but both experimental and computational characterization of their spectroscopic properties is difficult. We provide and compare results from 13 DFT and ab initio computational methods for up to 25 excited states of a paradigm system, the V N C B defect in hexagonal boron nitride (h-BN). Studied include include: (i) potentially catastrophic effects for computational methods arising from the multi-reference nature of the closed-shell and open-shell states of the defect, which intrinsically involves broken chemical bonds, (ii) differing results from DFT and time-dependent DFT (TDDFT) calculations, (iii) comparison of cluster models to periodic-slab models of the defect, (iv) the starkly differing effects of nuclear relaxation on the various electronic states as broken bonds try to heal that control the widths of photoabsorption and photoemission spectra, (v) the effect of zero-point energy and entropy on free-energy differences, (vi) defect-localized and conduction/valence band transition natures, and (vii) strategies needed to ensure that the lowest-energy state of a defect can be computationally identified. Averaged state-energy differences of 0.3 eV are found between CCSD(T) and MRCI energies, with thermal effects on free energies sometimes also being of this order. However, DFT-based methods can perform very poorly. Simple generalized-gradient functionals like PBE fail at the most basic level and should never be applied to defect states. Hybrid functionals like HSE06 work very well for excitations within the triplet manifold of the defect, with an accuracy equivalent to or perhaps exceeding the accuracy of the ab initio methods used. However, HSE06 underestimates triplet state energies by on average 0.7 eV compared to closed-shell singlet states, while open-shell singlet states are predicted to be too low in energy by 1.0 eV. This leads to miss-assignment of the ground state of the V N C B defect. Long-range corrected functionals like CAM-B3LYP are shown to work much better and to represent the current entry level for DFT calculations on defects. As significant differences between cluster and periodic-slab models are also found, the widespread implementation of such functionals in periodic codes is in urgent need.

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Section: Introductionmentioning

confidence: 99%

Understanding and Calibrating Density-Functional-Theory Calculations Describing the Energy and Spectroscopy of Defect Sites in Hexagonal Boron Nitride

Reimers

Ali

Kobayashi

et al. 2018

J. Chem. Theory Comput.

145

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show abstract

“…The III-V compounds are important semiconductors and the corresponding low-dimensional phases are becoming a focus of research. [7][8][9][10][11][12] Hexagonal-AlN (h-AlN) has attracted much attention. [13][14][15][16][17] The properties of h-AlN, such as the geometry, electronic structure and magnetic properties, can be tuned by absorbing or doping.…”

Section: Introductionmentioning

confidence: 99%

First-principles calculations of 5d atoms doped hexagonal-AlN sheets: Geometry, magnetic property and the influence of symmetry and symmetry-breaking on the electronic structure

Zhang¹,

Zhou²,

Zhao³

et al. 2014

Chinese Phys. B

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The geometry, electronic structure and magnetic property of the hexagonal AlN (h-AlN) sheet doped by 5d atoms (Lu, Hf, Ta, W, Re, Os, Ir, Pt, Au and Hg) are investigated by first-principles calculations based on the density functional theory. The influence of symmetry and symmetry-breaking is also studied. There are two types of local symmetries of the doped systems: C 3v and D 3h . The symmetry will deviate from exact C 3v and D 3h for some particular dopants after optimization. The total magnetic moments of the doped systems are 0µ B for Lu, Ta and Ir; 1µ B for Hf, W, Pt and Hg; 2µ B for Re and Au; and 3µ B for Os and Al-vacancy. The total densities of state are presented, where impurity energy levels exist. The impurity energy levels and total magnetic moments can be explained by the splitting of 5d orbitals or molecular orbitals under different symmetries.

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“…Many theoretical attempts have been made to study all kinds of possible defects in hBN so far . Early theoretical works mainly focused on studying the stability and structural properties of hBN sheets accommodating local defects, as well as their electronic and magnetic properties [129][130][131][132][133][134][135][136][137][138][139][140][141][142][143][144]. Further investigations clarified that some defect families exhibit deep band gaps levels [145,146], and more theoretical researches on these 'deep-level' defects have sprung up after observations of experimental SPEs in 2016 .…”

Section: Theoretical Investigationsmentioning

confidence: 99%

Spin-active defects in hexagonal boron nitride

Liu¹,

Guo²,

Yu³

et al. 2022

Mater. Quantum. Technol.

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Quantum technology grown out of quantum information theory, including quantum communication, quantum computation and quantum sensing, not only provides powerful research tools for numerous fields, but also is expected to go to civilian use in the future. Solid-state spin-active defects are one of promising platforms for quantum technology, and the host materials include three-dimensional diamond and silicon carbide, and the emerging two-dimensional hexagonal boron nitride (hBN) and transition-metal dichalcogenides. In this review, we will focus on the spin defects in hBN, and summarize theoretical and experimental progresses made in understanding properties of these spin defects. In particular, the combination of theoretical prediction and experimental verification is highlighted. We also discuss the future advantages and challenges of solid-state spins in hBN on the path towards quantum information applications.

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First-principles calculations of h-BN monolayers by doping with oxygen and sulfur

Cited by 11 publications

References 26 publications

Understanding and Calibrating Density-Functional-Theory Calculations Describing the Energy and Spectroscopy of Defect Sites in Hexagonal Boron Nitride

Understanding and Calibrating Density-Functional-Theory Calculations Describing the Energy and Spectroscopy of Defect Sites in Hexagonal Boron Nitride

First-principles calculations of 5d atoms doped hexagonal-AlN sheets: Geometry, magnetic property and the influence of symmetry and symmetry-breaking on the electronic structure

Spin-active defects in hexagonal boron nitride

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