Nitrogen-vacancy (NV) centers in diamond are pivotal for quantum sensing and information processing due to the exceptional spin and optical properties at ambient conditions. In this study, the synthesis of NV centers in nitrogen-rich diamond was systematically investigated using highly charged Argon ions (${\mathrm{Ar}}^{7+}$ at 1.89 MeV and ${\mathrm{Ar}}^{11+}$ at 2.97 MeV) combined with vacuum annealing. The results demonstrate that NV center production is nonmonotonically dependent on implantation fluence, with an optimized yield achieved at a moderate fluence of approximately ${10}^{13}$ ions/cm². Molecular dynamics simulations elucidate the microscopic evolution of vacancy generation, NV formation, and the vacancy cluster formation at excessive fluence. Furthermore, the spatial inhomogeneity of NV distribution near irradiation boundaries and unirradiated areas is mainly attributed to ion scattering effects and beam scanning during implantation. These findings provide a mechanistic understanding and practical guidelines for optimizing NV center fabrication via heavy-ion irradiation for quantum applications.

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• Quantum information theory