Intercalation phenomena in two-dimensional hybrid perovskites featuring discrete free volume elements

Abstract

Two-dimensional hybrid perovskites combine the exceptional optoelectronic properties of inorganic semiconductors with the expansive diversity of organic materials. While these organic ligands offer the opportunity to introduce new functionality to tailor the properties of the hybrid, their persistence within the architecture limits the extent of modulation in response to external stimuli. Here, we show using density functional theory that 2D hybrid perovskites assembled with mixtures of organic ligands to create free volume elements within the gallery space render the hybrids amenable to intercalation by organic small molecules. Though these intercalants produce relatively small changes in the materials architecture, their presence has a pronounced effect on the optoelectronic properties of two-dimensional L₂PbI₄ perovskites. Thus, an intriguing chemical space emerges for configuring customizable responsive materials using intercalation phenomena. We can envision on that basis new technologies exploiting those traits for selective or reversible detection of organic analytes.