Tailoring structure–property relationships in metal halide perovskites at an atomistic level
Lead Research Organisation:
UNIVERSITY OF OXFORD
Abstract
Hybrid metal-halide perovskites have made remarkable progress as thin-film semiconductors over the past decade. Solar cells based on these materials now reach certified power conversion efficiencies over 26% for single junction and 33% for tandem devices with silicon. In parallel, promising research has demonstrated efficient light-emitting diodes and photodetectors. These materials thus emerge as exciting tools for tackling climate change and energy security, some of the greatest challenges to be faced by humanity over the coming century. However, some challenges remain to be addressed, including long-term stability, and semiconductor quality across the full bandgap range. Material microstructure has become the critical parameter here, influencing charge-carrier transport and lifetimes, as well as ionic motion and material stability, through crystallographic defects and interfaces. Understanding and tailoring microstructure and defects in thin films will thus be the key to advances in perovskite device performance and stability.
The overarching vision for this project is to provide a step-change in this area, by establishing structure-property relationships in hybrid metal-halide semiconductors at an atomic-resolution level, uncovering causal links of their microstructure with optoelectronic properties and stability. These advances will be accomplished through a co-ordinated and well-interlinked collaborative programme bringing together a team of leading experts in advanced electron microscopy imaging, first-principles modelling, metal halide semiconductor thin-film and device fabrication, and experimental analysis of optoelectronic properties. We will deploy a cutting-edge combinatorial approach, correlating atomic-scale resolution imaging and multiscale defect mapping approaches with macroscopic analytical experiments and first-principles calculations revealing causal links between material microstructure, electronic properties and degradation pathways. This programme will generate vital progress in a number of critical areas, revealing directly at an atomic level the effects of stoichiometric imbalances and impurity phases, grain boundaries and defects, on macroscopic optoelectronic properties and material stability.
This work is urgent and timely: until recently, direct and reliable atomic-scale imaging of metal-halide perovskites in their relevant thin-films state had been prevented by their hybrid and soft nature which easily led to damage under electron beams used in high-resolution microscopy. Recent research, including ground-breaking advances by our team, has managed to overcome these obstacles through careful tuning of experimental parameters and analysis techniques. This places us in an ideal position to provide, for the first time, fully deterministic links between atomic-scale structure and macroscopic properties across the class of metal halide semiconductors, in order to realise their full potential in terms of performance and stability.
This project will be highly beneficial to society and the environment by enabling step-change improvements in next-generation semiconductors for high-efficiency photovoltaic and light-emitting devices. Such advances are critical to address climate change and energy security, and have the potential to open massive export markets for the UK, creating economic growth, jobs and future wealth. In addition, the outputs of this project will benefit a wide range of scientists, including those working in the industrial materials sector, stimulating research and development. The new insights gained on atomic-scale microstructure of metal halide semiconductors and the novel design rules for microstructure optimization will boost the development of ultra-efficient devices for our transition to net-zero carbon emissions. The new combinatorial methodologies developed and applied will trigger a wave of novel characterisation development, linking microscopic atomic-level information with macroscopic materials properties through accelerated analysis. This programme will thus also provide broader blue-prints for next-generation materials optimization approaches.
The overarching vision for this project is to provide a step-change in this area, by establishing structure-property relationships in hybrid metal-halide semiconductors at an atomic-resolution level, uncovering causal links of their microstructure with optoelectronic properties and stability. These advances will be accomplished through a co-ordinated and well-interlinked collaborative programme bringing together a team of leading experts in advanced electron microscopy imaging, first-principles modelling, metal halide semiconductor thin-film and device fabrication, and experimental analysis of optoelectronic properties. We will deploy a cutting-edge combinatorial approach, correlating atomic-scale resolution imaging and multiscale defect mapping approaches with macroscopic analytical experiments and first-principles calculations revealing causal links between material microstructure, electronic properties and degradation pathways. This programme will generate vital progress in a number of critical areas, revealing directly at an atomic level the effects of stoichiometric imbalances and impurity phases, grain boundaries and defects, on macroscopic optoelectronic properties and material stability.
This work is urgent and timely: until recently, direct and reliable atomic-scale imaging of metal-halide perovskites in their relevant thin-films state had been prevented by their hybrid and soft nature which easily led to damage under electron beams used in high-resolution microscopy. Recent research, including ground-breaking advances by our team, has managed to overcome these obstacles through careful tuning of experimental parameters and analysis techniques. This places us in an ideal position to provide, for the first time, fully deterministic links between atomic-scale structure and macroscopic properties across the class of metal halide semiconductors, in order to realise their full potential in terms of performance and stability.
This project will be highly beneficial to society and the environment by enabling step-change improvements in next-generation semiconductors for high-efficiency photovoltaic and light-emitting devices. Such advances are critical to address climate change and energy security, and have the potential to open massive export markets for the UK, creating economic growth, jobs and future wealth. In addition, the outputs of this project will benefit a wide range of scientists, including those working in the industrial materials sector, stimulating research and development. The new insights gained on atomic-scale microstructure of metal halide semiconductors and the novel design rules for microstructure optimization will boost the development of ultra-efficient devices for our transition to net-zero carbon emissions. The new combinatorial methodologies developed and applied will trigger a wave of novel characterisation development, linking microscopic atomic-level information with macroscopic materials properties through accelerated analysis. This programme will thus also provide broader blue-prints for next-generation materials optimization approaches.