Prediction and Synthesis of a Selenide Perovskite for Optoelectronics

Abstract

The advent of halide perovskites in recent years has opened an avenue for redeveloping perovskite materials as semiconductors. In the quest for semiconducting perovskites, chalcogenides, which exhibit higher stability than their halide siblings and often direct band gaps for optoelectronics, have attracted more and more attention. So far, functional chalcogenide perovskites have been exclusively sulfides. Here, employing first-principles calculations and the criterion of phase stability in addition to the commonly used thermodynamic and dynamical criteria, we precisely predict the existence of LaScSe3 as a thermodynamically stable selenide perovskite, which is validated by our experimental synthesis. Combining hybrid functional and many-body quasi-particle (G0W0 and Bethe–Salpeter equation) calculations, we predict that LaScSe3 is a direct-gap semiconductor having the band gap in the green-to-blue region and capable of p- and n-type bipolar doping, potentially for optoelectronic applications.

Enhancing the inherent stability of perovskite solar cells through chalcogenide-halide combinations

“…In addition, in 2023, Zhang et al discovered that LaScSe 3 is a thermodynamically stable selenide perovskite through the first principles calculation and accurate prediction of phase stability standard, and successfully verified this in subsequent experimental synthesis. 107…”

Solution processed metal chalcogenide semiconductors for inorganic thin film photovoltaics

“…167–169 Generally, most observed and predicted chalcogenide perovskites have sulfide anions, but a selenide perovskite has been found as well. 170…”

Moderate temperature sulfurization and selenization of highly stable metal oxides: an opportunity for chalcogenide perovskites

“…Chalcogenide perovskites generally contain a sulfide anion; however, select selenide perovskites have been synthesized. 1–3 Most of the known chalcogenide perovskites are made of alkaline earth metals, early transition metals, and metals found in the lanthanide and actinide series. 1,4 Compared with the late-transition metals and post-transition elements that make up many of the traditional semiconductors, the metals that make up chalcogenide perovskites are highly reactive towards oxygen sources and tend to be highly thermodynamically stable as metal oxides.…”