Ion Migration in Two-Dimensional Organic-Inorganic Hybrid Perovskite Heterostructures: Interface Evolution, Migration Mechanisms and Device Implications.

Two-dimensional organic-inorganic hybrid perovskite (2D-OIHP) heterostructures provide a versatile platform for crystal engineering because their composition, dimensionality, excitonic structure and interfacial energy alignment can be tuned at the molecular level. However, the same ionic softness that enables facile chemical transformation also leads to ion migration under thermal, electrical and optical stimuli. In 2D-OIHP heterostructures, ion migration is not only a degradation pathway; it determines whether a heterointerface remains sharp, becomes compositionally graded, evolves into a mixed-halide alloy, or forms a bias-programmed functional junction. This review summarizes recent progress in understanding ion migration in 2D-OIHP-based heterostructures, with emphasis on migration species, driving forces, pathways and interface evolution. We first classify representative fabrication strategies according to the initial interface profiles they generate. We then discuss thermally driven in-plane and out-of-plane halide migration, spacer-cation engineering for suppressing interdiffusion, and electric-field-induced directional migration in functional devices. Finally, we extract design rules and unresolved challenges for achieving stable, sharp or dynamically programmable perovskite heterostructures. The aim is to provide a mechanistic framework for using ion migration as both a stability criterion and a crystal-engineering tool in layered hybrid perovskites.