Defects and crystallinity control of perovskite films for light-emitting diodes

Metal halide perovskites are promising materials for the fabrication of cost-effective and highperformance light-emitting diodes (LEDs), due to their solution processability, high photoluminescence quantum efficiencies (PLQEs) and excellent charge transport properties. Importantly, perovskite LEDs show ultra-pure emission color, which is better than that of the state-of-the-art quantum dot LEDs (QLEDs) and organic LEDs (OLEDs), demonstrating a bright application potential for realizing vivid natural colors display in the future. In this thesis, we first incorporate natural molecules, e.g. deoxyribonucleic acid (DNA), to passivate FAPbI3 perovskite films. We notice that the existence of carbonyl and amide groups within DNA are important for efficient passivation of perovskite films. Combining the knowledge, we further introduce amino-functionalized molecules into perovskite films and achieve significantly improved efficiency of 21.6 %, which is a record external quantum efficiency (EQE) of perovskite LEDs. We reveal that by weakening the hydrogen bond strength between passivation molecules and organic cations, the interaction between passivation amino groups and defects improves, contributing to more efficient passivation. We also notice that the underlying substrates play important roles on the film quality of perovskite and the device performance of the ensuing LEDs. Here, we reveal that efficient deprotonation of the undesirable organic cations (Methylammonium (MA+) or Formamidinium (FA+)) by a metal oxide interlayer, e.g. ZnO, with a high isoelectric point, is critical to promote the transition from intermediate phases to highly emissive perovskites. We reveal synergistic effects of precursor stoichiometry and interfacial reactions for high-performance perovskite LEDs, and establish useful guidelines for rational device optimisation. With the knowledge we obtain from the deprotonation process, we further push the EL emission from near-infrared (NIR) (around 800 nm) region to deep red emission (around 700 nm) via cation exchange process between cesium (Cs+) and FA+, which promotes enhanced crystallization of the perovskite films and devices performance simultaneously. Intensive efforts in the perovskite community have pushed the EQEs of perovskite LEDs to over 20 %for green, red and NIR emission region. However, it is still a long way to go before their practical applications. We believe that efficient control of both the defects and crystallinity of the perovskite films through rational materials development and interfacial modifications is important for the development of perovskite optoelectronic devices. In addition, both our findings on the perovskite film quality control are universal and provide insights to promote the development of perovskites (especially the hybrid ones containing organic components) for the applications of other optoelectronic devices