DFT study of the role and possible contribution of defects to lithium metasilicate [formula omitted] luminescence

Abstract

Lithium metasilicate (Li2SiO3) has recently been shown to display outstanding stimulated luminescence properties, which are governed by defects and/or impurities. Here, the possible contribution and character of native point and complex defects to stimulated luminescence of lithium metasilicate have been investigated employing calculations based on the density functional theory (DFT). Under high concentrations of acceptor defects, isolated lithium interstitials were found to be the defects with the lowest formation energy (0.41 eV) but it is shown that they cannot contribute to luminescence. On the other hand, Oi−2 are the most favorable and stable defects under high concentrations of donor defects. F-centers and oxygen peroxides were identified as first- and second-order processes of point defects, which would explain experimental observations in the literature. Bridging oxygen vacancies were shown to introduce shallow electron traps able to trap up to four electrons. On the contrary, non-bridging oxygen vacancies lead to the formation of deep color centers with the capability of trapping up to two carriers/center, which could be the final state for the radiative process of luminescence. These results provide guidance for the interpretation of experimental measurements of luminescence.