The fields of photovoltaics, photodetection and light emission have seen tremendous activity in recent years with the advent of hybrid organic-inorganic perovskites. Yet, there have been far fewer reports of perovskite-based field-effect transistors. The lateral and interfacial transport requirements of transistors make them particularly vulnerable to surface contamination and defects rife in polycrystalline films and bulk single crystals. Here, we demonstrate a spatially-confined inverse temperature crystallization strategy which synthesizes micrometre-thin single crystals of methylammonium lead halide perovskites MAPbX3 (X = Cl, Br, I) with sub-nanometer surface roughness and very low surface contamination. These benefit the integration of MAPbX3 crystals into ambipolar transistors and yield record, room-temperature field-effect mobility up to 4.7 and 1.5 cm2 V−1 s−1 in p and n channel devices respectively, with 104 to 105 on-off ratio and low turn-on voltages. This work paves the way for integrating hybrid perovskite crystals into printed, flexible and transparent electronics.

Organolead trihalide perovskites have attracted significant attention for optoelectronic applications due to their excellent physical properties in the past decade. Generally, both grain boundaries in perovskite films and the device structure play key roles in determining the device performance, especially for horizontal‐structured device. Here, the first optimized vertical‐structured photodetector with the perovskite single crystal MAPbBr3 as the light absorber and graphene as the transport layer is shown. The hybrid device combines strong photoabsorption characteristics of perovskite and high carrier mobility of flexible graphene, exhibits excellent photoresponse performance with high photoresponsivity (≈1017.1 A W−1) and high photodetectivity (≈2.02 × 1013 Jones) in a low light intensity (0.66 mW cm−2) under the actuations of 3 V bias and laser irradiation at 532 nm. In particular, an ultrahigh photoconductive gain of ≈2.37 × 103 is attained because of fast charge transfer in the graphene and large recombination lifetime in the perovskite single crystal. The vertical architecture combining perovskite crystal with highly conductive graphene offers opportunities to fulfill the synergistic effect of perovskite and 2D materials, is thus promising for developing high‐performance electronic and optoelectronic devices.

Despite its extensive research in photovoltaics and light emitting diodes, the charge transport properties of all‐inorganic perovskite cesium lead bromide (CsPbBr3) remain elusive. Clarification of the intrinsic charge transport of this perovskite material is highly desirable, which will help to understand its working mechanism and fabricate high performance electronic devices. Here, it is demonstrated that the phototransistors based on CsPbBr3 microplates show anomalous ambipolar transport characteristics at room temperature. The hole mobility shows light dependence, while the electron mobility is identical under various light incidence. The hole mobility increases from 0.02 cm2 V−1 s−1 (in dark conditions) to 0.34 cm2 V−1 s−1 (50 mW cm−2); while the threshold voltage is shifted by 14 V when electron is the majority charge carrier. The anomalous transport behavior can be attributed to the photovoltaic and photoconductive effects. Moreover, the device shows photoresponsivity and detectivity up to 110 mA W−1 and 4.5 × 1013 Jones, respectively, under 532 nm laser illumination. This research unveils the charge transport mechanism of CsPbBr3 perovskite, provides more evidence and will thus contribute to the perovskite electronic and optoelectronic researches.

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Defect density is one of the most significant characteristics of perovskite single crystals (PSCs) that determines their optical and electrical properties, but few strategies are available to tune this property. Here, we demonstrate that voltage regulation is an efficient method to tune defect density, as well as the optical and electrical properties of PSCs. A three-step carrier transport model of MAPbBr3 PSCs is proposed to explore the defect regulation mechanism and carrier transport dynamics via an applied bias. Dynamic and steady-state photoluminescence measurements subsequently show that the surface defect density, average carrier lifetime, and photoluminescence intensity can be efficiently tuned by the applied bias. In particular, when the regulation voltage is 20 V (electrical poling intensity is 0.167 V μm−1), the surface defect density of MAPbBr3 PSCs is reduced by 24.27%, the carrier lifetime is prolonged by 32.04%, and the PL intensity is increased by 112.96%. Furthermore, a voltage-regulated MAPbBr3 PSC memristor device shows an adjustable multiresistance, weak ion migration effect and greatly enhanced device stability. Voltage regulation is a promising engineering technique for developing advanced perovskite optoelectronic devices.

Grains and grain boundaries play key roles in determining halide perovskite‐based optoelectronic device performance. Halide perovskite monocrystalline solids with large grains, smaller grain boundaries, and uniform surface morphology improve charge transfer and collection, suppress recombination loss, and thus are highly favorable for developing efficient solar cells. To date, strategies of synthesizing high‐quality thin monocrystals (TMCs) for solar cell applications are still limited. Here, by combining the antisolvent vapor‐assisted crystallization and space‐confinement strategies, high‐quality millimeter sized TMCs of methylammonium lead iodide (MAPbI3) perovskites with controlled thickness from tens of nanometers to several micrometers have been fabricated. The solar cells based on these MAPbI3 TMCs show power conversion efficiency (PCE) of 20.1% which is significantly improved compared to their polycrystalline counterparts (PCE) of 17.3%. The MAPbI3 TMCs show large grain size, uniform surface morphology, high hole mobility (up to 142 cm2 V−1 s−1), as well as low trap (defect) densities. These properties suggest that TMCs can effectively suppress the radiative and nonradiative recombination loss, thus provide a promising way for maximizing the efficiency of perovskite solar cells.

Abstract:The thermally-induced self-healing behavior of polymer coatings consists of two steps, i.e., gap closure and crack repair. In addition, the polymer coatings with thermally-induced self-healing capability are expected to show satisfied properties to ensure the application. Here, four epoxy coatings with dense irreversible Network I, dense reversible Network II based on a Diels-Alder (DA) reaction, loose irreversible Network III, as well as partially irreversible and partially reversible Network IV were prepared, respectively. The dense irreversible Network I showed an evident gap closure upon heating, while the crack still existed at the high temperature. The dense reversible Network II presented good self-healing upon direct heating at a high temperature of 150 • C, leading to the quick gap closure in 40 s and subsequent crack disappearance in 80 s. The loose irreversible Network III showed negligible crack variations upon heating, while the partially reversible and partially irreversible Network IV showed quick gap closure as well but only partial crack disappearance. Besides, the coating with the reversible Network II based on the DA reaction not only presented good self-healing capability but also possessed the satisfied mechanical properties and the best electrochemical corrosion property, ensuring its further exploitation and potential practical applications.

Nonradiative recombination loss is a key process that determines the performance of perovskite solar cells, and how to control it is significant for the research and development of perovskites. Generally, traditional chemical modification/passivation methods are complicated and prone to secondary contamination. Herein, femtosecond (fs) laser polishing as a promising technique is demonstrated to ameliorate the surface of perovskite films, reduce nonradiative recombination loss, and improve solar cell performance. The high‐intensity fs laser pulses can remove around 20 nm‐thick perovskite top layer through an ionization process, help to decrease the grain boundary density, and enlarge the grain size of perovskite films after recrystallization. It is believed that fs laser polishing is a time‐effective and highly precise technique that is suitable for large‐scale device production, thus will trigger more applications in optoelectronics.