First-principles study of the formation of Group-IV--vacancy color centers in diamond

Abstract

$XV$ ($X$ is Si, Ge, Sn, or Pb, and $V$ is the carbon vacancy) color centers are promising platforms for quantum computing and quantum information science due to their favorable optical and spin properties. They are commonly fabricated by ion implantation, which inevitably introduces vacancies and carbon self-interstitials (C$_i$) into the lattice. However, the microscopic formation mechanism remains unclear, limiting the yield and stability of $XV$ centers. Here, first-principles calculations are conducted to systematically investigate the roles of $V$ and C$_i$ in $XV$ formation. We find that $XV$ formation is energetically favorable, with large binding energies and low diffusion barriers. Nevertheless, $XV$ readily captures C$_i$ to form substitutional defect $X_s$, or captures an additional $V$ to form the complex $XV_2$. Charge transition levels show that oppositely charged reactants never meet in these reactions, and that Coulomb repulsion blocks them only when both reactants carry charges of the same sign, which for the capture of C$_i$ requires strongly n- or p-type conditions. These competing defect reactions destabilize the split-vacancy configuration and could account for the low formation yield of $XV$ centers, so that they appear at concentrations well below those expected from the implanted dose. Our results elucidate the microscopic origin of this intrinsic instability and suggest that Fermi-level control may suppress defect conversions and stabilize the split-vacancy configuration.