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In situ cyclized polyacrylonitrile (CPAN) is developed to replace n‐type metal oxide semiconductors (TiO2 or SnO2) as an electron selective layer (ESL) for highly efficient and stable n‐i‐p perovskite solar cells (PSCs). The CPAN layer is fabricated via facile in situ cyclization reaction of polyacrylonitrile (PAN) coated on a conducting glass substrate. The CPAN layer is robust and insoluble in common solvents, and possesses n‐type semiconductor properties with a high electron mobility of 4.13×10−3 cm2 V−1 s−1. With the CPAN as an ESL, the PSC affords a power conversion efficiency (PCE) of 23.12 %, which is the highest for the n‐i‐p PSCs with organic ESLs. Moreover, the device with the CPAN layer holds superior operational stability, maintaining over 90 % of their initial efficiency after 500 h continuous light soaking. These results confirm that the CPAN layer would be a desirable low‐cost and efficient ESL for n‐i‐p PSCs and other photoelectronic devices with high performance and stability. [ABSTRACT FROM AUTHOR]

2D chiral perovskite has greatly boosted the development of optoelectronic devices, ranging from nonlinear optics, spintronics, and ferroelectrics to energy harvesting devices. Despite circularly polarized light (CPL) detection based on chiral perovskite has been achieved, the environmental humidity‐, ultraviolet (UV), and temperature‐induced structural degradation and its large electro‐phonon coupling restrict its commercial application. Here, this study first realizes polymerized chiral perovskite single‐crystal films by combining in situ cross‐linking polymerization with the space‐confined crystallization method. Compared with uncross‐linked chiral perovskites, cross‐linked chiral perovskites exhibit enhanced crystallinity and lattice rigidity, yielding high‐performance circularly polarized photodetectors with a maximum anisotropy factor of 0.22, the responsivity of 1.6 A W−1, and detectivity of 2.17 × 1013 Jones. In addition, flexible circularly polarized photodetectors with extremely high mechanical stability are also realized originating from the polymer‐like behavior of cross‐linked chiral perovskite single‐crystal films. This study opens up new avenues to further enhance the performance and stability of portable and wearable devices based on chiral perovskites. [ABSTRACT FROM AUTHOR]

2D organic semiconductor crystals (2D OSCs) are vital for high‐performance electronic and optoelectronic devices owing to their unique material merits. However, it is still challenging to fabricate high‐quality and large‐scale ultrathin 2D OSCs with controllable molecular layers due to the disordered molecular deposition and uncontrollable mass transport in solution‐processing fabrication. Here, a vapor‐induced meniscus modulating strategy for preparing unidirectional and stable Marangoni flow to guide contactless meniscus evolution is reported, which ensures uniform mass transport and ordered molecular deposition to achieve high‐quality ultrathin 2D OSCs. Both the surface tension difference and the substrate wettability are critical to meniscus formation, which results in various meniscus deformation states and film morphologies. Based on the optimized vapor‐solvent system, ultrathin 2D OSCs of C8‐BTBT with precise layer definition are prepared controllably. The discrepancies in liquid film height and solute concentration are decisive in controlling the molecular scale thickness ranging from mono to a few layers. Moreover, the layer‐dependent electronic and optoelectronic properties of the ultrathin films are systematically investigated. Notably, high‐performance polarization‐sensitive solar‐blind photodetectors are achieved with a dichroic ratio of photocurrent up to 2.26, and the corresponding polarimetric image sensor exhibits superior solar‐blind polarization imaging capability thanks to the high crystalline quality. [ABSTRACT FROM AUTHOR]

Highlights: Optimizing the current collectors with rGO and the addition of CNT in PPy, and the structural pulverization is prevented significantly. Areal capacitances of 65.9 to 70 mF cm−2 are achieved for PPy-CNT@rGO microsupercapacitors (MSCs) with 79% capacitance retention after 10,000 cycles. The MSC-derived capacitive micro-strain sensor is capable of biosignals detection. The micro strain sensor is capable of detecting wide levels of applied strain with short response/recovery time and excellent reliability. Conducting polymers have achieved remarkable attentions owing to their exclusive characteristics, for instance, electrical conductivity, high ionic conductivity, visual transparency, and mechanical tractability. Surface and nanostructure engineering of conjugated conducting polymers offers an exceptional pathway to facilitate their implementation in a variety of scientific claims, comprising energy storage and production devices, flexible and wearable optoelectronic devices. A two-step tactic to assemble high-performance polypyrrole (PPy)-based microsupercapacitor (MSC) is utilized by transforming the current collectors to suppress structural pulverization and increase the adhesion of PPy, and then electrochemical co-deposition of PPy-CNT nanostructures on rGO@Au current collectors is performed. The resulting fine patterned MSC conveyed a high areal capacitance of 65.9 mF cm−2 (at a current density of 0.1 mA cm−2), an exceptional cycling performance of retaining 79% capacitance after 10,000 charge/discharge cycles at 5 mA cm−2. Benefiting from the intermediate graphene, current collector free PPy-CNT@rGO flexible MSC is produced by a facile transfer method on a flexible substrate, which delivered an areal capacitance of 70.25 mF cm−2 at 0.1 mA cm−2 and retained 46% of the initial capacitance at a current density of 1.0 mA cm−2. The flexible MSC is utilized as a skin compatible capacitive micro-strain sensor with excellent electromechanochemical characteristics. [ABSTRACT FROM AUTHOR]

Advancing hole transport layers (HTL) to realize large‐area, flexible, and high‐performance perovskite solar cells (PSCs) is one of the most challenging issues for its commercialization. Here, a self‐assembled gradient Ti3C2Tx MXene incorporated PEDOT:PSS HTL is demonstrated to achieve high‐performance large‐area PSCs by establishing half‐caramelization‐based glucose‐induced MXene redistribution. Through this process, the Ti3C2Tx MXene nanosheets are spontaneously dispersed and redistributed at the top region of HTL to form the unique gradient distribution structure composed of MXene:Glucose:PEDOT:PSS (MG‐PEDOT). These results show that the MG‐PEDOT HTL not only offers favorable energy level alignment and efficient charge extraction, but also improves the film quality of perovskite layer featuring enlarged grain size, lower trap density, and longer carrier lifetime. Consequently, the power conversion efficiency (PCE) of the flexible device based on MG‐PEDOT HTL is increased by 36% compared to that of pristine PEDOT:PSS HTL. Meanwhile, the flexible perovskite solar minimodule (15 cm2 area) using MG‐PEDOT HTL achieve a PCE of 17.06%. The encapsulated modules show remarkable long‐term storage stability at 85 °C in ambient air (≈90% efficiency retention after 1200 h) and enhanced operational lifetime (≈90% efficiency retention after 200 h). This new approach shows a promising future of the self‐assembled HTLs for developing optoelectronic devices. [ABSTRACT FROM AUTHOR]

Driven by the Internet of Everything, one of the main goals in human–computer interaction is to achieve intuitive, effortless, and easy‐to‐learn communication. Thus, senseless optoelectronic devices with high response performance under ambient environment have an extensive application space in improving the interfacing between users and computers. Herein, a concept of wearable perovskite‐based shadow recognition sensor is demonstrated for ambient and nonobtrusive human–computer interaction. The multidimensional ordered nucleation and growth of perovskite crystals are promoted by introducing the self‐driving effect of liquid crystal (LC) oligomers. The resulted LC‐doped perovskite film (LC‐PVK) with micrometer‐sized grains can output relatively high photocurrent under indoor ambient light (≈500 lux). The LC‐based device exhibits over a hundred times of on–off ratio and fast response of millisecond level even after storage for more than 1200 h. The device also shows an ultratrace Pb2+ leakage of 1.02 μg L−1 in water, and still retains more than 90% of the photocurrent intensity after thousands of bending strains. Accordingly, a novel human–computer interaction is achieved by identifying external action commands with the recognition of shadows, which can provide a "haptic" perception for robots. [ABSTRACT FROM AUTHOR]

Metal halide perovskite, an emerging photosensitive semiconductor, has been widely employed in solar cells, light‐emitting diodes, photodetectors, and lasers owing to its excellent photophysical properties and simple solution preparation processing. However, as a photoactive layer, the higher refractive index and thinner thickness of perovskite film can cause reflection and transmission at the interface, and confine the emitted light within devices, resulting in the poor incident photon absorption and emitted photon extraction. In addition, the intrinsic brittleness of perovskite material restricts its potential applications in flexible optoelectronics. Therefore, great effort has been put into micro‐nano structured perovskite optoelectronics, and the reported reviews mainly focus on the fabrication process of micro‐nano patterned perovskite. Herein, the functionalities of micro‐nano structures in optoelectronics, including improving the light trapping, light extraction, light modulation, carrier dynamics, mechanical robustness, and other novel functionalities, are comprehensively reviewed. The specific applications of these functionalities in perovskite‐based optoelectronic devices are then discussed in detail to provide a better understanding of the photophysical properties of micro‐nano structure functionalized optoelectronics. Finally, promising strategies to promote the multifunctional commercial applications of micro‐nano structured perovskite optoelectronics are provided. [ABSTRACT FROM AUTHOR]

Perovskites as promising photovoltaic materials have been widely investigated due to their excellent photoelectric properties. Perovskite optoelectronic devices have been applied in fields of portable energy, light monitors, image sensors, etc. In recent years, wearable perovskite optoelectronic devices have been developed for their advantages of flexibility, stretchability, and light weight. In this review, the latest development of flexible and wearable perovskite optoelectronic devices is summarized. First, the preparation methods of optoelectronic devices are introduced, especially focusing on the large‐scale fabrication. Then the latest advances of various flexible devices are presented. In particular, the stability and safety of wearable devices, as well as the impact factors and corresponding solutions are discussed. Finally, the challenges for practical applications are put forward and discussed. [ABSTRACT FROM AUTHOR]

Extensive applications for photodetectors have led to demand for high‐responsivity polarization‐sensitive light detection. Inspired by the elaborate architecture of butterfly Papilio paris, a 1D nanograting bonded porous 2D photonic crystal perovskite photodetector (G‐PC‐PD) using a commercial DVD master and 2D crystalline colloidal arrays template was fabricated. The coupling effect from grating diffraction and reflection of the PC stopband renders the enhanced light harvesting of G‐PC‐PD. The porous scaffold and nanoimprinting process afford a highly crystalline perovskite film. White light responsivity and detectivity of G‐PC‐PD are up to 12.67 A W−1 and 3.22×1013 Jones (6∼7 times that of a pristine perovskite photodetector). The highly ordered nanograting arrays of G‐PC‐PD enable polarization‐sensitive light detection with a rate of −0.72 nA deg−1. This hierarchical perovskite integrated nanograting and 2D PC architecture opens a new avenue to high‐performance optoelectronic devices. [ABSTRACT FROM AUTHOR]

A systematic understanding of perovskite single crystal is critical for the development of high-performance functional devices. We outline the synthesis strategies, unique characteristics, and optoelectronic applications of perovskite single crystals with diverse dimensions, including 0D perovskite QDs, 1D micro/nanowires arrays, 2D micro/nanoplates arrays and single-crystal films, and 3D micro/nanoscale single-crystal structures, providing guidelines for the application of integrated devices. [Display omitted] Lead halide perovskite single crystals have emerged as promising candidates for high-performance optoelectronic devices because of their superior optoelectronic properties. To date, much literature has reported the fabrication of various perovskite single-crystal structures. However, it still lacks effective rationalization and a comprehensive understanding of the relationship between the structural characteristics and functional properties of the perovskite single crystals, which is of great significance for fabricating perovskite single crystals-based high-performance optoelectronic devices. In this review, we give a comprehensive overview of the synthesis of perovskite single crystals with diverse dimensions, including 0D perovskite quantum dots (QDs), 1D micro/nanowires, 2D micro/nanoplates and single-crystal thin films (SCTFs), and 3D micro/nanoscale single-crystal structures. The relationship between the dimensional structure and properties of the perovskite single crystals is discussed in detail. Dimensional requirements for different optoelectronic applications are systematically summarized. Finally, perspectives on remaining challenges and future opportunities are highlighted. [ABSTRACT FROM AUTHOR]