Dimensionality-Driven Charge Stabilization of Group-IV Color Centers in Diamond Ultrathin Films
Neutral group-IV vacancy (XV, X = Si, Ge, Sn, and Pb) centers in diamond are emerging solid-state spin-photon interfaces because of their favorable spin coherence and inversion symmetry-protected optical transitions. However, stabilizing their neutral charge state typically requires stringent Fermi-level engineering in high purity boron-doped diamond, which poses significant materials-growth challenges. Here, we demonstrate that dimensional confinement in diamane provides an alternative route to charge-state stabilization without intentional doping. Using first-principles calculations, we show that quantum confinement and surface termination cooperatively tune the host band gap and shift the occupied defect states upward from the valence-band edge, thereby enlarging the thermodynamic stability window of the neutral charge state and suppressing valence-band assisted excitation pathways. We further reveal that the thickness and surface termination of diamane enable systematic tuning of the electronic structure, zero-field splitting, and spin-orbit coupling of XV centers while largely preserving their optical transition energies. Among the structures considered, hydrogenated diamane offers the most favorable balance between charge-state stability and magneto-optical performance. More broadly, our findings establish dimensional confinement as a general strategy for engineering the charge, optical, and spin properties of solid-state quantum defects.