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Origin and designing of large ground-state zero-field splitting of color centers in diamond

MetadataDetails
Publication Date2024-07-08
JournalPhysical review. B./Physical review. B
AuthorsChen Qiu, Han-Pu Liang, Hui Deng, Su‐Huai Wei
InstitutionsInstitute of Semiconductors, Beijing Computational Science Research Center

In diamond, the pivotal factor for quantum applications involving color centers hinges on extending the spin coherence time through a larger ground-state zero-field splitting (ZFS). Experimental observations indicate a correlation between the atomic number and the increasing of the ground-state ZFS of group-IV centers. Yet, the physical origin underlying the impurity-modulated ground-state ZFS remains insufficiently elucidated. In this study, utilizing density-functional theory and group analysis, we illustrate that the origin of the correlation between the ground-state ZFS in group-IV centers and the atomic number of impurity atoms, arises from the synergistic interplay of large atomic numbers and the extent of $p\text{\ensuremath{-}}d$ orbital hybridization. Simultaneously, our investigation identifies that the ground-state of group-IVB centers originates from a robust $p\text{\ensuremath{-}}p$ hybridization between impurity atom and divacancy. This interaction results in ground-state ZFS of 7728 GHz for $\mathrm{Hf}{V}^{\ensuremath{-}}$ centers, nearly doubling the experimentally observed value found in the largest $\mathrm{Pb}{V}^{\ensuremath{-}}$ centers. Our study, therefore, provides profound insights into the origins of the impurity-modulated ground-state ZFS, offering a promising pathway towards achieving larger ground-state ZFS of color centers.