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<p>Diamond defects are among the most promising qubits. Modeling their properties through accurate quantum mechanical simulations can further their development into robust units of information. We use the recently developed capped density functional embedding theory (capped-DFET) with the multiconfigurational <i>n</i>-electron valence second-order perturbation theory to characterize the electronic excitation energies for different spin manifolds of the well-characterized negatively charged substitutional N defect adjacent to a vacancy (V<sub>C</sub>) in diamond (N<sub>C</sub>V<sub>C</sub><sup>−</sup>). We successfully reproduce vertical excitation energies for both triplet and singlet states of N<sub>C</sub>V<sub>C</sub><sup>−</sup> with errors &lt; 0.1 eV. Unlike other embedding methods, capped-DFET exhibits robust predictions that are approximately independent of the embedded cluster size: it only requires a cluster to contain the defect atoms and their nearest neighbors (as small as a 40-atom capped cluster). Furthermore, our method is free from slowly converging Coulomb interactions between charged defects, and thus also only weakly dependent on supercell size.</p>

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Optical properties of a diamond NV color center from capped embedded multiconfigurational correlated wavefunction theory

  • 期刊论文

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  • 发表日期：

    2026年2月6日

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  • John Mark P. Martirez

摘要

Diamond defects are among the most promising qubits. Modeling their properties through accurate quantum mechanical simulations can further their development into robust units of information. We use the recently developed capped density functional embedding theory (capped-DFET) with the multiconfigurational n-electron valence second-order perturbation theory to characterize the electronic excitation energies for different spin manifolds of the well-characterized negatively charged substitutional N defect adjacent to a vacancy (VC) in diamond (NCVC−). We successfully reproduce vertical excitation energies for both triplet and singlet states of NCVC− with errors < 0.1 eV. Unlike other embedding methods, capped-DFET exhibits robust predictions that are approximately independent of the embedded cluster size: it only requires a cluster to contain the defect atoms and their nearest neighbors (as small as a 40-atom capped cluster). Furthermore, our method is free from slowly converging Coulomb interactions between charged defects, and thus also only weakly dependent on supercell size.