On-Shelf and Operational Decay Dynamics of Self-Healing Quasi-Two-Dimensional Perovskite Light-Emitting Devices

J Phys Chem Lett. 2024 Feb 22;15(7):2039-2048. doi: 10.1021/acs.jpclett.3c03596. Epub 2024 Feb 13.

Abstract

Currently, the external quantum efficiency (EQE) performance of perovskite light-emitting diodes (PeLEDs) is approaching its theoretical limit. The main drawback of PeLEDs is their stability. Ion migration in the perovskite layer is one of the main causes of the operational decomposition of PeLEDs. Here, we find that butylammonium-based quasi-two-dimensional (quasi-2D) PeLEDs show self-healing ability, revealing the existence of ion migration in the fabricated perovskite layer. Then, on the basis of the analysis of ∼170 operational decay EQE curves, patterns of on-shelf and operational decay in self-healing quasi-2D PeLEDs have been identified. The uneven distributions of resistance on the perovskite film surface are proposed to cause secondary electric fields. The electroluminescent scintillation in certain regions results in fluctuating electroluminescence of PeLEDs, further proving the existence of microcosmic steric ion movement under secondary electric fields. Our work explores the decay patterns of self-healing PeLEDs and highlights the impact of steric ion movements on the decay processes of PeLEDs.