Photoluminescence Mapping of Mobile and Fixed Defects in Halide Perovskite Films

TL;DR

This paper introduces a localized, contact-free photoluminescence mapping technique to measure and distinguish mobile and immobile ionic defects in halide perovskite films, advancing understanding of ionic transport in these materials.

Contribution

It develops a localized IMPLS method to quantify lateral ionic diffusion and separate defect types in perovskite films, overcoming limitations of electrical measurement techniques.

Findings

IMPLS-derived ionic diffusion coefficients match literature values.

IMPLS can spatially distinguish mobile and immobile defects.

The method provides a contact-free way to analyze ionic transport.

Abstract

Metal halide perovskites exhibit coupled electronic and ionic properties that determine their photovoltaic performance and operational stability. Understanding and quantifying ionic transport are therefore essential for advancing perovskite optoelectronics. Conventional electrical methods such as impedance spectroscopy require fully integrated devices, and their interpretation is often complicated by interfacial and contact effects, limiting the ability to isolate intrinsic ionic behavior. Here, a localized adaptation of intensity-modulated photoluminescence spectroscopy (IMPLS) is utilized to optically probe lateral ionic transport in perovskite films. The frequency-dependent photoluminescence response is measured under controlled carrier injection levels and correlated with the photoluminescence quantum yield (PLQY). The proposed diffusion model indicates that mobile ionic defects laterally migrate from high light intensity regions, giving rise to characteristic photoluminescence modulations. Ionic diffusion coefficients extracted from IMPLS agree well with literature values obtained from electrical measurements. Importantly, IMPLS mapping separates mobile and immobile defect contributions through a defect contrast coefficient (DCC), which quantifies the normalized difference between the area-averaged photoluminescence intensity and phase data. This work ultimately demonstrates that localized IMPLS provides a contact-free means to extract lateral ion diffusion coefficients while spatially distinguishing defect types across the sample.