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Thiocyanate-Stabilized Pseudo-cubic Perovskite CH(NH<sub>2</sub>)<sub>2</sub>PbI<sub>3</sub> from Coincident Columnar Defect Lattices

Takuya Ohmi, Iain W. H. Oswald, James R. Neilson, Nikolaj Roth, Shunta Nishioka, Kazuhiko Maeda, Kotaro Fujii, Masatomo Yashima, Masaki Azuma, Takafumi Yamamoto

2023Journal of the American Chemical Society12 citationsDOI

Abstract

α-FAPbI 3 (FA + = CH(NH 2 ) 2 + ) with a cubic perovskite structure is promising for photophysical applications. However, α-FAPbI 3 is metastable at room temperature, and it transforms to the δ-phase at a certain period of time at room temperature. Herein, we report a thiocyanate-stabilized pseudo-cubic perovskite FAPbI 3 with ordered columnar defects (α′-phase). This compound has a √5 a p × √5 a p × a p tetragonal unit cell ( a p: cell parameter of primitive perovskite cell) with a band gap of 1.91 eV. It is stable at room temperature in a dry atmosphere. Furthermore, the presence of the α′-phase in a mixed sample with the δ-phase drastically reduces the δ-to-α transition temperature measured on heating, suggesting the reduction of the nucleation energy of the α-phase or thermodynamic stabilization of the α-phase through epitaxy. The defect-ordered pattern in the α′-phase forms a coincidence-site lattice at the twinned boundary of the single crystals, thus hinting at an epitaxy- or strain-based mechanism of α-phase formation and/or stabilization. In this study, we developed a new strategy to control defects in halide perovskites and provided new insight into the stabilization of α-FAPbI 3 by pseudo-halide and grain boundary engineering.

Topics & Concepts

ChemistryHalideTetragonal crystal systemPerovskite (structure)NucleationCrystallographyMetastabilityPhase (matter)Grain boundaryEpitaxyCrystal structureInorganic chemistryMicrostructureLayer (electronics)Organic chemistryPerovskite Materials and ApplicationsSolid-state spectroscopy and crystallographyCrystal Structures and Properties
Thiocyanate-Stabilized Pseudo-cubic Perovskite CH(NH<sub>2</sub>)<sub>2</sub>PbI<sub>3</sub> from Coincident Columnar Defect Lattices | Litcius