Abstract

Halide perovskite is one of the most promising semiconducting materials in a variety of fields such as solar cells, photodetectors, and light-emitting diodes. Lead halide perovskite single crystals featuring long diffusion length, high carrier mobility, large light absorption coefficient and low defect density, have been attracting increasing attention. Fundamental study of the intrinsic nature keeps revealing the superior optoelectrical properties of perovskite single crystals over their polycrystalline thin film counterparts, but to date, the device performance lags behind. The best power conversion efficiency (PCE) of single crystal-based solar cells is 21.9%, falling behind that of polycrystalline thin film solar cells (25.2%). The oversized thickness, defective surfaces, and difficulties in depositing functional layers, hinder the application of halide perovskite single crystals in optoelectronic devices. Efforts have been made to synthesize large-area single crystalline thin films directly on conductive substrates and apply defect engineering approaches to improve the surface properties. This review starts from a comprehensive introduction of the optoelectrical properties of perovskite single crystals. Then, the synthesis methods for high-quality bulk crystals and single-crystalline thin films are introduced and compared, followed by a systematic review of their optoelectronic applications including solar cells, photodetectors, and X-ray detectors. The challenges and strategical approaches for high-performance applications are summarized at the end with a brief outlook on future work.

Highlights

  • In recent years, there has been blooming development in hybrid organic–inorganic halide perovskite materials as they possess outstanding photoelectronic properties and cost-effective low-temperature solution processability

  • Perovskite single crystals stand out as one of the most promising semiconductor materials to be applied in optoelectronic applications

  • Various synthesis methods have been developed, In summary, perovskite single crystals stand out as one of the most promising semiconductor aiming at harvesting high-quality and large-size single crystals

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Summary

Introduction

There has been blooming development in hybrid organic–inorganic halide perovskite materials as they possess outstanding photoelectronic properties and cost-effective low-temperature solution processability. In comparison with polycrystalline phase thin films, single crystal halide perovskite materials show superior properties in various optoelectronic applications such as solar cells, photodetectors, and light-emitting diodes. The inefficient carrier transport and collection behaviour due to the mismatch of the relatively short diffusion length and large thickness limit the application of single crystals for high-performance devices in a vertical structure. A 20 μm-thick MAPbI3 (MA+ : methylammonium, CH3 NH3 + ) monocrystalline made by space-limited low-temperature crystallisation was fabricated into inverted-structure solar cells with a PCE of 21.9% [26], narrowing the gap between the single crystals and polycrystalline thin films. Critical discussion on the existing challenges and corresponding solutions will shed significant insight into exploring strategic approaches to further promote the research of single crystals and their device applications

Properties of Single Crystals
Crystal
Synthesis Methods of Perovskite Single Crystals
Method
Inverse
Schematic
Perovskite Single Crystals for Photodetectors
NH large‐area
Synthesis Process
Surface
11. Real‐space
Interface
H5 groups
Regulation
Findings
Summary

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