Pressure Regulating Self-Trapped States toward Remarkable Emission Enhancement of Zero-Dimensional Lead-Free Halides Nanocrystals

Copper(I)-based halides have recently attracted increasing attention as a substitute for lead halides, owing to their nontoxicity, abundance, unique structure, and optoelectric properties. However, exploring an effective strategy to further improve their optical activities and revealing structure-optical property relationships still remain a great concern. Here, by using high pressure technique, a remarkable enhancement of self-trapped exciton (STE) emission associated with the energy exchange between multiple self-trapped states in zero-dimensional lead-free halide Cs3Cu2I5 NCs is successfully achieved. Furthermore, high-pressure processing endows the piezochromism of Cs3Cu2I5 NCs by experiencing a white light and a strong purple light emission, which is able to be stabilized at near-ambient pressure. The distortion of [Cu2I5] clusters composing of tetrahedral [CuI4] and trigonal planar [CuI3] and the decreased Cu-Cu distance between the adjacent Cu-I tetrahedron and triangle are responsible for the significant STEs emission enhancement under high pressure. The experiments combined with first-principles calculations not only shed light on the structure-optical property relationships of [Cu2I5] clusters halide, but also provide guidance for improving emission intensity that is highly desirable in solid-state lighting applications.