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arXiv · 2505.11240

Nitrogen-vacancy centre in lonsdaleite: a novel nanoscale sensor?

Anjay Manian·Mitchell O. de Vries·Daniel Stavrevski·Qiang Sun·Salvy P. Russo·Andrew D. Greentree
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Abstract

Hexagonal diamond, often called lonsdaleite, is an exotic allotrope of carbon, predicted to be harder than cubic (conventional) diamond with a wider bandgap. Due to its pure sp$^3$ bonded lattice, it should be expected to host sub-bandgap defect centres (colour centres). Here we perform \textit{ab initio} modeling of nitrogen-vacancy (NV) colour centres in hexagonal diamond nanocrystals; for both the neutral and negatively charged species (NV$^0$ and NV$^-$). We identify three distinct configurations for the NV center: two of which are analogous to NV in diamond, and one which is a configuration that can only exist in the hexagonal form. The diamond-like NV systems comprise three symmetry equivalent centers which reside on the same carbon plane, and one defect that is split across two planes and replaces a carbon-carbon bond. There is an additional NV centre where the N and V each have four nearest neighbour carbon atoms. The presence of this latter configuration would provide an unambiguous determination of the hexagonal nature of lonsdaleite. Quantum chemical analysis show all derivatives to be thermochemically stable, and each with their own unique photophysical properties, spectral profiles, and magneto-optical characteristics. By assuming that the ground state properties of the NV$^-$ in hexagonal diamond are comparable to those of NV$^-$ in cubic diamond, albeit with increased strain, we predict ground state fine structure splitting for two of the centres of 2.74~GHz and 4.56~MHz, compared with 2.87~GHz for cubic diamond. The possibility of optically detected magnetic resonance with NV$^-$ in lonsdaleite would provide a new carbon-based quantum sensing system, and an unambiguous method to resolve outstanding issues around the structure of lonsdaleite as hexagonal diamond.

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Anjay Manian, Mitchell O. de Vries, Daniel Stavrevski, Qiang Sun, Salvy P. Russo, Andrew D. Greentree. 2025-05-16. Nitrogen-vacancy centre in lonsdaleite: a novel nanoscale sensor?. https://arxiv.org/abs/2505.11240

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