High‐Performance Flexible Photodetectors based on High‐Quality Perovskite Thin Films by a Vapor–Solution Method

Organometal halide perovskites are new light‐harvesting materials for lightweight and flexible optoelectronic devices due to their excellent optoelectronic properties and low‐temperature process capability. However, the preparation of high‐quality perovskite films on flexible substrates has still been a great challenge to date. Here, a novel vapor–solution method is developed to achieve uniform and pinhole‐free organometal halide perovskite films on flexible indium tin oxide/poly(ethylene terephthalate) substrates. Based on the as‐prepared high‐quality perovskite thin films, high‐performance flexible photodetectors (PDs) are constructed, which display a nR value of 81 A W^?1 at a low working voltage of 1 V, three orders higher than that of previously reported flexible perovskite thin‐film PDs. In addition, these flexible PDs exhibit excellent flexural stability and durability under various bending situations with their optoelectronic performance well retained. This breakthrough on the growth of high‐quality perovskite thin films opens up a new avenue to develop high‐performance flexible optoelectronic devices.     

Controlling Nucleation and Growth of Metal Halide Perovskite Thin Films for High‐Efficiency Perovskite Solar Cells

Metal halide perovskite thin films can be crystallized via a broad range of solution‐based routes. However, the quality of the final films is strongly dependent upon small changes in solution composition and processing parameters. Here, this study demonstrates that a fractional substitution of PbCl₂ with PbI₂ in the 3CH₃NH₃I:PbCl₂ mixed‐halide starting solution has a profound influence upon the ensuing thin‐film crystallization. The presence of PbI₂ in the precursor induces a uniform distribution of regular quadrilateral‐shaped CH₃NH₃PbI₃ perovskite crystals in as‐cast films, which subsequently grow to form pinhole‐free perovskite films with highly crystalline domains. With this new formulation of 3CH₃NH₃I:0.98PbCl₂:0.02PbI₂, this study achieves a 19.1% current–voltage measured power conversion efficiency and a 17.2% stabilized power output in regular planar heterojunction solar cells.     

Molecular Glass Resists as High‐Resolution Patterning Materials

The success of the semiconductor industry is based on the ability to fabricate hundreds of millions of devices on a single chip. In order to fulfill the ever‐shrinking feature sizes, the industry requires new patternable materials in order to operate in the sub‐50 nm regime. Molecular glass (MG) resists are a new type of patterning material that has gained considerable attention over the past few years. This Research News article describes the chemical and structural aspects of MGs as well as important concepts of MG resist design. We also highlight some of the recent advances in high‐resolution patterning capabilities with next‐generation imaging tools.     

Templated Solid‐State Dewetting of Thin Silicon Films

Thin film dewetting can be efficiently exploited for the implementation of functionalized surfaces over very large scales. Although the formation of sub‐micrometer sized crystals via solid‐state dewetting represents a viable method for the fabrication of quantum dots and optical meta‐surfaces, there are several limitations related to the intrinsic features of dewetting in a crystalline medium. Disordered spatial organization, size, and shape fluctuations are relevant issues not properly addressed so far. This study reports on the deterministic nucleation and precise positioning of Si‐ and SiGe‐based nanocrystals by templated solid‐state dewetting of thin silicon films. The dewetting dynamics is guided by pattern size and shape taking full control over number, size, shape, and relative position of the particles (islands dimensions and relative distances are in the hundreds nm range and fluctuate ≈11% for the volumes and ≈5% for the positioning).     

Perovskite Light‐Emitting Diodes with Improved Outcoupling Using a High‐Index Contrast Nanoarray

Organic–inorganic hybrid perovskite light‐emitting diodes (PeLEDs) are promising for next‐generation optoelectronic devices due to their potential to achieve high color purity, efficiency, and brightness. Although the external quantum efficiency (EQE) of PeLEDs has recently surpassed 20%, various strategies are being pursued to increase EQE further and reduce the EQE gap compared to other LED technologies. A key point to further boost EQE of PeLEDs is linked to the high refractive index of the perovskite emissive layer, leading to optical losses of more than 70% of emitted photons. Here, it is demonstrated that a randomly distributed nanohole array with high‐index contrast can effectively enhance outcoupling efficiency in PeLEDs. Based on a comprehensive optical analysis on the perovskite thin film and outcoupling structure, it is confirmed that the nanohole array effectively distributes light into the substrate for improved outcoupling, allowing for 1.64 times higher light extraction. As a result, highly efficient red/near‐infrared PeLEDs with a peak EQE of 14.6% are demonstrated.     

High‐Performance Solution‐Processed Organo‐Metal Halide Perovskite Unipolar Resistive Memory Devices in a Cross‐Bar Array Structure

Resistive random access memories can potentially open a niche area in memory technology applications by combining the advantages of the long endurance of dynamic random‐access memory and the long retention time of flash memories. Recently, resistive memory devices based on organo‐metal halide perovskite materials have demonstrated outstanding memory properties, such as a low‐voltage operation and a high ON/OFF ratio; such properties are essential requirements for low power consumption in developing practical memory devices. In this study, a nonhalide lead source is employed to deposit perovskite films via a simple single‐step spin‐coating method for fabricating unipolar resistive memory devices in a cross‐bar array architecture. These unipolar perovskite memory devices achieve a high ON/OFF ratio up to 10⁸ with a relatively low operation voltage, a large endurance, and long retention times. The high‐yield device fabrication based on the solution‐process demonstrated here will be a step toward achieving low‐cost and high‐density practical perovskite memory devices.     

Low‐Temperature Soft‐Cover Deposition of Uniform Large‐Scale Perovskite Films for High‐Performance Solar Cells

Large‐scale high‐quality perovskite thin films are crucial to produce high‐performance perovskite solar cells. However, for perovskite films fabricated by solvent‐rich processes, film uniformity can be prevented by convection during thermal evaporation of the solvent. Here, a scalable low‐temperature soft‐cover deposition (LT‐SCD) method is presented, where the thermal convection‐induced defects in perovskite films are eliminated through a strategy of surface tension relaxation. Compact, homogeneous, and convection‐induced‐defects‐free perovskite films are obtained on an area of 12 cm², which enables a power conversion efficiency (PCE) of 15.5% on a solar cell with an area of 5 cm². This is the highest efficiency at this large cell area. A PCE of 15.3% is also obtained on a flexible perovskite solar cell deposited on the polyethylene terephthalate substrate owing to the advantage of presented low‐temperature processing. Hence, the present LT‐SCD technology provides a new non‐spin‐coating route to the deposition of large‐area uniform perovskite films for both rigid and flexible perovskite devices.     

High‐Resolution,Parallel Patterning of Nanoparticles via an Ion‐Induced Focusing Mask

An ion‐induced focusing mask under the simultaneous injection of ions and charged aerosols generates invisible electrostatic lenses around each opening, through which charged nanoparticles are convergently guided without depositing on the mask surface. The sizes of the created features become significantly smaller than those of the mask openings due to the focusing capability. It is not only demonstrated that material‐independent nanoparticles including proteins can be patterned as an ordered array on any surface regardless of the conductive, nonconductive, or flexible nature of the substrate, but also that the array density can be increased. Highly sensitive gas sensors based on these focused nanoparticle patterns are fabricated via the concept.     

High‐Performance Single‐Crystalline Perovskite Thin‐Film Photodetector

The best performing modern optoelectronic devices rely on single‐crystalline thin‐film (SC‐TF) semiconductors grown epitaxially. The emerging halide perovskites, which can be synthesized via low‐cost solution‐based methods, have achieved substantial success in various optoelectronic devices including solar cells, lasers, light‐emitting diodes, and photodetectors. However, to date, the performance of these perovskite devices based on polycrystalline thin‐film active layers lags behind the epitaxially grown semiconductor devices. Here, a photodetector based on SC‐TF perovskite active layer is reported with a record performance of a 50 million gain, 70 GHz gain‐bandwidth product, and a 100‐photon level detection limit at 180 Hz modulation bandwidth, which as far as we know are the highest values among all the reported perovskite photodetectors. The superior performance of the device originates from replacing polycrystalline thin film by a thickness‐optimized SC‐TF with much higher mobility and longer recombination time. The results indicate that high‐performance perovskite devices based on SC‐TF may become competitive in modern optoelectronics.     

Polarized Ferroelectric Polymers for High‐Performance Perovskite Solar Cells

In hybrid organic–inorganic lead halide perovskite solar cells, the energy loss is strongly associated with nonradiative recombination in the perovskite layer and at the cell interfaces. Here, a simple but effective strategy is developed to improve the cell performance of perovskite solar cells via the combination of internal doping by a ferroelectric polymer and external control by an electric field. A group of polarized ferroelectric (PFE) polymers are doped into the methylammonium lead iodide (MAPbI₃) layer and/or inserted between the perovskite and the hole‐transporting layers to enhance the build‐in field (BIF), improve the crystallization of MAPbI₃, and regulate the nonradiative recombination in perovskite solar cells. The PFE polymer‐doped MAPbI₃ shows an orderly arrangement of MA⁺ cations, resulting in a preferred growth orientation of polycrystalline perovskite films with reduced trap states. In addition, the BIF is enhanced by the widened depletion region in the device. As an interfacial dipole layer, the PFE polymer plays a critical role in increasing the BIF. This combined effect leads to a substantial reduction in voltage loss of 0.14 V due to the efficient suppression of nonradiative recombination. Consequently, the resulting perovskite solar cells present a power conversion efficiency of 21.38% with a high open‐circuit voltage of 1.14 V.