Organic-inorganic mixed halide perovskites have emerged as an excellent class of materials with a unique combination of optoelectronic properties, suitable for a plethora of applications ranging from solar cells to light-emitting diodes and photoelectrochemical devices. Recent works have showcased hybrid perovskites for electronic applications through improvements in materials design, processing, and device stability. Herein, a comprehensive up-to-date review is presented on hybrid perovskite electronics with a focus on transistors and memories. These applications are supported by the fundamental material properties of hybrid perovskite semiconductors such as tunable bandgap, ambipolar charge transport, reasonable mobility, defect characteristics, and solution processability, which are highlighted first. Then, recent progresses on perovskite-based transistors are reviewed, covering aspects of fabrication process, patterning techniques, contact engineering, 2D versus 3D material selection, and device performance. Furthermore, applications of perovskites in nonvolatile memories and artificial synaptic devices are presented. The ambient instability of hybrid perovskites and the strategies to tackle this bottleneck are also discussed. Finally, an outlook and opportunities to develop perovskite-based electronics as a competitive and feasible technology are highlighted.

Halide Perovskites: A New Era of Solution-Processed Electronics.

Recently, metal-halide perovskites have emerged as promising materials for photodetector (PD) applications owing to their superior optoelectronic properties, such as ambipolar charge transport characteristics, high carrier mobility, and so on. In the past few years, rapid progress in lead-based perovskite PDs has been witnessed. However, the critical environmental instability and lead-toxicity seriously hinder their further applications and commercialization. Therefore, searching for environmentally stable and lead-free halide perovskites (LFHPs) to address the above hurdles is certainly a worthwhile subject. In this review, we present a comprehensive overview of currently explored LFHPs with an emphasis on their crystal structures, optoelectronic properties, synthesis and modification methods, as well as the PD applications. LFHPs are classified into four categories according to the replacement strategies of Pb2+, including AB(II)X3, A3B(III)2X9, A2B(I)B(III)′X6, and newly-emerging perovskite derivatives. Then, we give a demonstration of the preliminary achievements and limitations in environment-friendly PDs based on such LFHPs and perovskite derivatives, and also discuss their applications in biological synapses, imaging, and X-ray detection. With the perspective of their properties and current challenges, we provide an outlook for future directions in this rapidly evolving field to achieve high-quality LFHPs and perovskite derivatives for a broader range of fundamental research and practical applications.

Recent advances toward environment-friendly photodetectors based on lead-free metal halide perovskites and perovskite derivatives.

The key to protect sensitive information stored in electronic memory devices from disclosure is to develop transient electronic devices that are capable of being destroyed quickly in an emergency. By using a highly water-soluble polythiophene-conjugated polyelectrolyte PTT-NMI+Br- as an active material, which was synthesized by the reaction of poly[thiophene-alt-4,4-bis(6-bromohexyl)-4H-cyclopenta(1,2-b:5,4-b')dithiophene] with N-methylimidazole, a flexible electronic device, Al/PTT-NMI+Br-/ITO-coated PET (ITO: indium tin oxide; PET: polyethylene terephthalate), is successfully fabricated. This device shows a typical nonvolatile rewritable resistive random access memory (RRAM) effect at a sweep voltage range of ±3 V and a history-dependent memristive switching performance at a small sweep voltage range of ±1 V. Both the learning/memorizing functions and the synaptic potentiation/depression of biological systems have been emulated. The switching mechanism for the PTT-NMI+Br--based electronic device may be highly associated with ion migration under bias. Once water is added to this device, it will be destructed rapidly within 20 s due to the dissolution of the active layer. This device is not only a typical transient device but can also be used for constructing conventional memristors with long-term stability after electronic packaging. Furthermore, the soluble active layer in the device can be easily recycled from its aqueous solution and reused for fabricating new transient memristors. This work offers a train of new thoughts for designing and constructing a neuromorphic computing system that can be quickly destroyed with water in the near future.

Water-Soluble Polythiophene-Conjugated Polyelectrolyte-Based Memristors for Transient Electronics.

Understanding photogenerated charge transport is critical to further improving the performance of perovskite‐based devices. In this study, the low‐defect perovskite CH3NH3PbX3 (X = Br or Cl) single crystals, which are an ideal platform for high‐quality optoelectronic devices, are fabricated to examine characteristics of photodetectors with electrodes with Au or Ag, and interlayer of TiO2. The transport mechanism of the photogenerated carriers in each device is elucidated by analysis of the current density–voltage curves under dark or a 405 nm of super‐bandgap illumination or a 640 nm of sub‐bandgap illumination. The photocurrent under the 405 nm illumination is improved under the hole‐dominant Au‐device of p‐type bromide crystals and the electron‐dominant Ag‐device of n‐type chloride crystals. The defect‐assisted excitation under 640 nm illumination is associated with generation of the holes with the defects located near the conduction band or the electrons with the valence band in each perovskite materials. With this conception, the responsivity of 0.07 A W−1, specific detectivity over 1011 Jones, and external quantum efficiency around 16% are obtained in the best performing devices. The present results suggest a promising strategy for designing efficient photodetectors using photogenerated and trap‐assisted photocarriers that contribute to enhanced photocurrent.

UV and Visible Photodetectors of MAPbBr3 and MAPbCl3 Perovskite Single Crystals via Single Photocarrier Transport Design

Organic-inorganic halide perovskites (OIHPs) have emerged as an active layer for resistive switching memory (RSM). Among various OIHPs, two-dimensional OIHPs are advantageous in RSMs because of their stability. This stability can be further improved using two-dimensional Dion-Jacobson OIHPs. Moreover, OIHP-based RSMs operated by the formation of halide-ion filaments are affected by grain boundaries because they can act as a shortcut for ion migration. Therefore, it is essential to control the grains in OIHPs for reliable memory operation. Here, we present RSMs using Dion-Jacobson OIHP with controlled grain sizes. The grain sizes of the OIHP are effectively controlled by adjusting the ratio of the N,N-dimethylformamide and dimethyl sulfoxide. The controlled grain sizes can modulate the paths for halide ion migration, which enables the change of the on/off ratio in RSM. In addition, cross-point array structure is essential for high-density memory applications. However, in the cross-point array structure, unwanted current flow through unselected memory cells can happen due to sneak-current paths, so it is necessary to suppress leakage current from neighboring cells by adopting selector devices. We demonstrate the application of selector devices to OIHP-based RSMs to prevent sneak current paths. These results provide the potential of OIHP for use in high-density memory applications.

Controlling the Grain Size of Dion-Jacobson-Phase Two-Dimensional Layered Perovskite for Memory Application.

Robust and Transient Write-Once-Read-Many-Times Memory Device Based on Hybrid Perovskite Film with Novel Room Temperature Molten Salt Solvent

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Robust and Transient Write-Once-Read-Many-Times Memory Device Based on Hybrid Perovskite Film with Novel Room Temperature Molten Salt Solvent