CsPbBr3 Perovskites: Theoretical and Experimental Investigation on Water-Assisted Transition From Nanowire Formation to Degradation

TL;DR

This study combines experiments and first-principles calculations to elucidate how water induces structural transitions and degradation in CsPbBr3 perovskites, revealing mechanisms behind their stability and breakdown.

Contribution

It provides a detailed atomistic understanding of water-driven structural evolution and degradation pathways in CsPbBr3 perovskites, integrating experimental observations with theoretical insights.

Findings

Water causes a two-step degradation process under UV light.

Formation of nanowire bundles enhances environmental stability.

Degradation results in PbBr2 and CsBr formation.

Abstract

Recent advances in colloidal synthesis methods have led to increased research focus on halide perovskites. Due to highly ionic crystal structure of perovskite materials, stability issue pops up especially against polar solvents such as water. In this study, we investigate water-driven structural evolution of CsPbBr3 by performing experiments and state-of-the-art first-principles calculations. It is seen that while optical image shows the gradual degradation of yellowish-colored CsPbBr3 structure under daylight, UV illumination reveals that the degradation of crystals takes place in two steps; transition from blue-emitting to green-emitting structure and and then transition from green-emitting phase to complete degradation. We found that as-synthesized CsPbBr3 NWs emit blue light under 254 nm UV source and before the degradation, first CsPbBr3 NWs undergoes a water-driven structural transition to form large bundles. It is also seen that formation of such bundles provide longer-term environmental stability. In addition theoretical calculations revealed how strong is the interaction of water molecules with ligands and surfaces of CsPbBr3 and provide atomistic-level explanation to transition from ligand-covered nanowires to bundle formation. Further interaction of green-light-emitting bundles with water causes complete degradation of CsPbBr3 and photoluminescence signal is entirely quenched. Moreover, Raman and XRD measurements revealed that completely degraded regions are decomposed to PbBr2 and CsBr precursors. We believe that findings of this study may provide further insight into the degradation mechanism of CsPbBr3 perovskite by water.