Point Defects Modeling Explains Multiple Sulfur Species in Sulfur-Doped Na₄(Al₃Si₃O₁₂)Cl Sodalite

Colorless Na4(Al3Si3O12)Cl sodalite exhibits the propensity to host sulfur atoms that give rise interesting optical properties. Namely, observed color, luminescence, and photochromism properties are commonly associated with presence of specific (Sn)x− species (n = 2 or 3; x 1 2) trapped in lattice concomitantly chlorine vacancies, when needed for charge balance. In this paper, we present a theoretical investigation native point defects some sulfur-based may form sodalite. DFT calculations were used simulate formation energies possible different states charge, together their relative transition energy levels concentrations. Our results unambiguously demonstrate ions easily replace chloride at various oxidation low cost. This study is also first one on defect full determination stability domain senary system (Na/Al/Si/O/Cl S).