Spin decontamination for magnetic dipolar coupling calculations: Application to high-spin molecules and solid-state spin qubits

Abstract

An accurate description of the two-electron density, crucial for magnetic coupling in spin systems, provides in general a major challenge for density functional theory calculations. It affects, e.g., the calculated zero-field splitting (ZFS) energies of spin qubits in semiconductors that frequently deviate significantly from experiment. In the present work (i) we propose an efficient and robust strategy to correct for spin contamination in both extended periodic and finite-size systems, (ii) verify its accuracy using model high-spin molecules, and finally (iii) apply the methodology to calculate accurate ZFS of spin qubits (NV${}^{-}$ centers, divacancies) in diamond and silicon carbide. The approach is shown to reduce the dependence on the used exchange-correlation functional to a minimum.

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Cited by in corpus (10)

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• Stability and electronic structure of NV centers at dislocation cores in diamond
• Influence of (N,H)-terminated surfaces on stability, hyperfine structure, and zero-field splitting of NV centers in diamond
• Influence of extended defects on the formation energy, the hyperfine structure, and the zero-field splitting of NV centers in diamond
• Temperature dependent spin-phonon coupling of boron-vacancy centers in hexagonal boron nitride
• 14N Hyperfine and nuclear interactions of axial and basal NV centers in 4H-SiC: A high frequency (94 GHz) ENDOR study
• Topological Defects in Semiconducting Carbon Nanotubes as Triplet Exciton Traps and Single-Photon Emitters
• First-principles computational methods for quantum defects in two-dimensional materials: A perspective
• Towards Identifying the PL6 Center in SiC: From First-Principles Screening to Hyperfine Validation of Competing Defect Candidates
• Spin-Phonon Relaxation of Boron-Vacancy Centers in Two-Dimensional Boron Nitride Polytypes