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

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journal contribution
posted on 2021-07-21, 15:37 authored by Adrien Stoliaroff, Romain Schira, Féodor Blumentritt, Emmanuel Fritsch, Stéphane Jobic, Camille Latouche
Colorless Na4(Al3Si3O12)Cl sodalite exhibits the propensity to host sulfur atoms that give rise to interesting optical properties. Namely, the observed color, the luminescence, and the photochromism properties are commonly associated with the presence of specific (Sn)x species (n = 2 or 3; x = 1 or 2) trapped in the host lattice concomitantly with chlorine vacancies, when needed for charge balance. In this paper, we present a theoretical investigation of the native point defects and some sulfur-based point defects that may form in sodalite. DFT calculations were used to simulate the formation energies of possible defects in different states of charge, together with their relative transition energy levels and concentrations. Our results unambiguously demonstrate that sulfur ions may easily replace chloride in sodalite at various oxidation states for a low energy cost. This study is also the first one on defect formation energy with a full determination of the stability domain on a senary system (Na/Al/Si/O/Cl and S).