Phase-Modulated Multidimensional Perovskites for High-Sensitivity Self-Powered UV Photodetectors

2D Ruddlesden-Popper perovskites (PVKs) have recently shown overwhelming potential in various optoelectronic devices on account of enhanced stability to their 3D counterparts. So far, regulating the phase distribution and orientation of 2D perovskite thin films remains challenging to achieve efficient charge transport. This work elucidates the balance struck between sufficient gradient sedimentation of perovskite colloids and less formation of small-n phases, which results in the layered alignment of phase compositions and thus in enhanced photoresponse. The solvent engineering strategy, together with the introduction of poly(3,4-ethylene-dioxythiophene):polystyrene sulfonate (PEDOT:PSS) and PC₇₁BM layer jointly contribute to outstanding self-powered performance of indium tin oxide/PEDOT:PSS/PVK/PC₇₁BM/Ag device, with a photocurrent of 18.4 µA and an on/off ratio up to 2800. The as-fabricated photodetector exhibits high sensitivity characteristics with the peak responsivity of 0.22 A W⁻¹ and the detectivity up to 1.3 × 10¹² Jones detected at UV-A region, outperforming most reported perovskite-based UV photodetectors and maintaining high stability over a wide spectrum ranging from UV to visible region. This discovery supplies deep insights into the control of ordered phases and crystallinity in quasi-2D perovskite films for high-performance optoelectronic devices.     

Flexible and Self-Powered Photodetector Arrays Based on All-Inorganic CsPbBr3 Quantum Dots

Flexible devices are garnering substantial interest owing to their potential for wearable and portable applications. Here, flexible and self-powered photodetector arrays based on all-inorganic perovskite quantum dots (QDs) are reported. CsBr/KBr-mediated CsPbBr₃ QDs possess improved surface morphology and crystallinity with reduced defect densities, in comparison with the pristine ones. Systematic material characterizations reveal enhanced carrier transport, photoluminescence efficiency, and carrier lifetime of the CsBr/KBr-mediated CsPbBr₃ QDs. Flexible photodetector arrays fabricated with an optimum CsBr/KBr treatment demonstrate a high open-circuit voltage of 1.3 V, responsivity of 10.1 A W⁻¹, specific detectivity of 9.35 × 10¹³ Jones, and on/off ratio up to ≈10⁴. Particularly, such performance is achieved under the self-powered operation mode. Furthermore, outstanding flexibility and electrical stability with negligible degradation after 1600 bending cycles (up to 60°) are demonstrated. More importantly, the flexible detector arrays exhibit uniform photoresponse distribution, which is of much significance for practical imaging systems, and thus promotes the practical deployment of perovskite products.     

Highly Efficient and Ultrasensitive Large‐Area Flexible Photodetector Based on Perovskite Nanowires

Hybrid organic–inorganic perovskites have shown exceptional semiconducting properties and microstructural versatility for inexpensive, solution‐processable photovoltaic and optoelectronic devices. In this work, an all‐solution‐based technique in ambient environment for highly sensitive and high‐speed flexible photodetectors using high crystal quality perovskite nanowires grown on Kapton substrate is presented. At 10 V, the optimized photodetector exhibits a responsivity as high as 0.62 A W^?1, a maximum specific detectivity of 7.3 × 10¹² cm Hz^1/2 W^?1, and a rise time of 227.2 µs. It also shows remarkable photocurrent stability even beyond 5000 bending cycles. Moreover, a deposition of poly(methyl methacrylate) (PMMA) as a protective layer on the perovskite yields significantly better stability under ambient air operation: the PMMA‐protected devices are stable for over 30 days. This work demonstrates a cost‐effective fabrication technique for high‐performance flexible photodetectors and opens opportunities for research advancements in broadband and large‐scale flexible perovskite‐based optoelectronic devices.     

Self‐Powered,Flexible, and Solution‐Processable Perovskite Photodetector Based on Low‐Cost Carbon Cloth

Flexible perovskite photodetectors are usually constructed on indium‐tin‐oxide‐coated polymer substrates, which are expensive, fragile, and not resistant to high temperature. Herein, for the first time, a high‐performance flexible perovskite photodetector is fabricated based on low‐cost carbon cloth via a facile solution processable strategy. In this device, perovskite microcrystal and Spiro‐OMeTAD (hole transporting material) blended film act as active materials for light detection, and carbon cloth serves as both a flexible substrate and a conductive electrode. The as‐fabricated photodetector shows a broad spectrum response from ultraviolet to near‐infrared light, high responsivity, fast response speed, long‐term stability, and self‐powered capability. Flexible devices show negligible degradation after several tens of bending cycles and at the extremely bending angle of 180°. This work promises a new technique to construct flexible, high‐performance photodetectors with low cost and self‐powered capability.     

Ultrahigh‐Performance Self‐Powered Flexible Double‐Twisted Fibrous Broadband Perovskite Photodetector

Self‐powered flexible photodetectors without an external power source can meet the demands of next‐generation portable and wearable nanodevices; however, the performance is far from satisfactory becuase of the limited match of flexible substrates and light‐sensitive materials with proper energy levels. Herein, a novel self‐powered flexible fiber‐shaped photodetector based on double‐twisted perovskite–TiO₂–carbon fiber and CuO–Cu₂O–Cu wire is designed and fabricated. The device shows an ultrahigh detectivity of 2.15 × 10¹³ Jones under the illumination of 800 nm light at zero bias. CuO–Cu₂O electron block bilayer extends response range of perovskite from 850 to 1050 nm and suppresses dark current down to 10^?11 A. The fast response speed of less than 200 ms is nearly invariable after dozens of cycles of bending at the extremely 90 bending angle, demonstrating excellent flexibility and bending stability. These parameters are comparable and even better than reported flexible and even rigid photodetectors. The present results suggest a promising strategy to design photodetectors with integrated function of self‐power, flexibility, and broadband response.     

Gradient Energy Band Driven High‐Performance Self‐Powered Perovskite/CdS Photodetector

Self‐powered photodetectors are highly desired to meet the great demand in applications of sensing, communication, and imaging. Manipulating the carrier separation and recombination is critical to achieve high performance. In this paper, a self‐powered photodetector based on the integrated gradient O‐doped CdS nanorod array and perovskite is presented. Through optimizing the degree of continuous built‐in band bending in the gradient‐O CdS, the photodetector demonstrates a remarkable detectivity of 2.1 × 10¹³ Jones. Under the self‐powered voltage mode, the responsivity can be as high as 0.48 A W^?1, and the rise and decay time are 0.54/2.21 ms. The comprehensive performance is comparable and even better than reported perovskite and other types of self‐powered photodetectors. The improved mechanism reveals that the gradient band bending promotes the photogenerated carrier transfer and hinders the recombination at the interface.     

High Performance and Stable All‐Inorganic Metal Halide Perovskite‐Based Photodetectors for Optical Communication Applications

Photodetectors are critical parts of an optical communication system for achieving efficient photoelectronic conversion of signals, and the response speed directly determines the bandwidth of the whole system. Metal halide perovskites, an emerging class of low‐cost solution‐processed semiconductors, exhibiting strong optical absorption, low trap states, and high carrier mobility, are widely investigated in photodetection applications. Herein, through optimizing the device engineering and film quality, high‐performance photodetectors based on all‐inorganic cesium lead halide perovskite (CsPbI_xBr_3–x), which simultaneously possess high sensitivity and fast response, are demonstrated. The optimized devices processed from CsPbIBr₂ perovskite show a practically measured detectable limit of about 21.5 pW cm^?2 and a fast response time of 20 ns, which are both among the highest reported device performance of perovskite‐based photodetectors. Moreover, the photodetectors exhibit outstanding long‐term environmental stability, with negligible degradation of the photoresponse property after 2000 h under ambient conditions. In addition, the resulting perovskite photodetector is successfully integrated into an optical communication system and its applications as an optical signal receiver on transmitting text and audio signals is demonstrated. The results suggest that all‐inorganic metal halide perovskite‐based photodetectors have great application potential for optical communication.     

Dual‐Phase CsPbBr3–CsPb2Br5 Perovskite Thin Films via Vapor Deposition for High‐Performance Rigid and Flexible Photodetectors

Inorganic perovskites with special semiconducting properties and structures have attracted great attention and are regarded as next generation candidates for optoelectronic devices. Herein, using a physical vapor deposition process with a controlled excess of PbBr₂, dual‐phase all‐inorganic perovskite composite CsPbBr₃–CsPb₂Br₅ thin films are prepared as light‐harvesting layers and incorporated in a photodetector (PD). The PD has a high responsivity and detectivity of 0.375 A W^?1 and 10¹¹ Jones, respectively, and a fast response time (from 10% to 90% of the maximum photocurrent) of ≈280 µs/640 µs. The device also shows an excellent stability in air for more than 65 d without encapsulation. Tetragonal CsPb₂Br₅ provides satisfactory passivation to reduce the recombination of the charge carriers, and with its lower free energy, it enhances the stability of the inorganic perovskite devices. Remarkably, the same inorganic perovskite photodetector is also highly flexible and exhibits an exceptional bending performance (>1000 cycles). These results highlight the great potential of dual‐phase inorganic perovskite films in the development of optoelectronic devices, especially for flexible device applications.     

Disentangling the Role of the SnO Layer on the Pyro-Phototronic Effect in ZnO-Based Self-Powered Photodetectors

Self-powered photodetectors (PDs) have been recognized as one of the developing trends of next-generation optoelectronic devices. Herein, it is shown that by introducing a thin layer of SnO film between the Si substrate and the ZnO film, the self-powered photodetector Al/Si/SnO/ZnO/ITO exhibits a stable and uniform violet sensing ability with high photoresponsivity and fast response. The SnO layer introduces a built-in electrostatic field to highly enhance the photocurrent by over 1000%. By analyzing energy diagrams of the p-n junction, the underlying physical mechanism of the self-powered violet PDs is carefully illustrated. A high photo-responsivity (R) of 93 mA W⁻¹ accompanied by a detectivity (D*) of 3.1 × 10¹⁰ Jones are observed under self-driven conditions, when the device is exposed to 405 nm excitation laser wavelength, with a laser power density of 36 mW cm⁻² and at a chopper frequency of 400 Hz. The Si/SnO/ZnO/ITO device shows an enhancement of 3067% in responsivity when compared to the Al/Si/ZnO/ITO. The photodetector holds an ultra-fast response of ≈ 2 µs, which is among the best self-powered photodetectors reported in the literature based on ZnO.     

Molecular Synergistic Passivation for Efficient Perovskite Solar Cells and Self-Powered Photodetectors

The interface between the perovskite and electron-transporting material is often treated for defect passivation to improve the photovoltaic performance of devices. A facile 4-Acetamidobenzoic acid (containing an acetamido, a carboxyl, and a benzene ring)-based molecular synergistic passivation (MSP) strategy is developed here to engineer the SnO_x/perovskite interface, in which dense SnO_x are prepared using an E-beam evaporation technology while the perovskite is deposited with vacuum flash evaporation deposition method. MSP engineering can synergistically passivate defects at the SnO_x/perovskite interface by coordinating with Sn⁴⁺ and Pb²⁺ with functional group  CO in the acetamido and carboxyl. The optimized solar cell devices can achieve the highest efficiency of 22.51% based on E-Beam deposited SnO_x and 23.29% based on solution-processed SnO₂, respectively, accompanied by excellent stability exceeding 3000 h. Further, the self-powered photodetectors exhibit a remarkably low dark current of 5.22 × 10⁻⁹ A cm⁻², a response of 0.53 A W⁻¹ at zero bias, a detection limit of 1.3 × 10¹³ Jones, and a linear dynamic range up to 80.4 dB. This work proposes a molecular synergistic passivation strategy to enhance the efficiency and responsivity of solar cells and self-powered photodetectors.     

Hybrid Organic–Inorganic Perovskite Photodetectors

Hybrid organic–inorganic perovskite materials garner enormous attention for a wide range of optoelectronic devices. Due to their attractive optical and electrical properties including high optical absorption coefficient, high carrier mobility, and long carrier diffusion length, perovskites have opened up a great opportunity for high performance photodetectors. This review aims to give a comprehensive summary of the significant results on perovskite‐based photodetectors, focusing on the relationship among the perovskite structures, device configurations, and photodetecting performances. An introduction of recent progress in various perovskite structure‐based photodetectors is provided. The emphasis is placed on the correlation between the perovskite structure and the device performance. Next, recent developments of bandgap‐tunable perovskite and hybrid photodetectors built from perovskite heterostructures are highlighted. Then, effective approaches to enhance the stability of perovskite photodetector are presented, followed by the introduction of flexible and self‐powered perovskite photodetectors. Finally, a summary of the previous results is given, and the major challenges that need to be addressed in the future are outlined. A comprehensive summary of the research status on perovskite photodetectors is hoped to push forward the development of this field.     

Direct Growth of Perovskite Crystals on Metallic Electrodes for High‐Performance Electronic and Optoelectronic Devices

Metal halide perovskite has attracted enhanced interest for its diverse electronic and optoelectronic applications. However, the fabrication of micro‐ or nanoscale crystalline perovskite functional devices remains a great challenge due to the fragility, solvent, and heat sensitivity of perovskite crystals. Here, a strategy is proposed to fabricate electronic and optoelectronic devices by directly growing perovskite crystals on microscale metallic structures in liquid phase. The well‐contacted perovskite/metal interfaces ensure these heterostructures serve as high‐performance field effect transistors (FETs) and excellent photodetector devices. When serving as an FET, the on/off ratio is as large as 10⁶ and the mobility reaches up to ≈2.3 cm² V^?1 s^?1. A photodetector is displayed with high photoconductive switching ratio of ≈10⁶ and short response time of ≈4 ms. Furthermore, the photoconductive response is proved to be band‐bending‐assisted separation of photoexcited carriers at the Schottky barrier of the silver and p‐type perovskites.     

A Highly Sensitive Single Crystal Perovskite–Graphene Hybrid Vertical Photodetector

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.     

Perovskite Single-Crystal Microwire-Array Photodetectors with Performance Stability beyond 1 Year

Compared with thin-film morphology, 1D perovskite structures such as micro/nanowires with fewer grain boundaries and lower defect density are very suitable for high-performance photodetectors with higher stability. Although the stability of perovskite microwire-based photodetectors has been substantially enhanced in comparison with that of photodetectors based on thin-film morphology, practical applications require further improvements to the stability before implementation. In this study, a template-assisted method is developed to prepare methylammonium lead bromide (MAPbBr₃) micro/nanowire structures, which are encapsulated in situ by a protective hydrophobic molecular layer. The combination of the protective layer, high crystalline quality, and highly ordered microstructures significantly improve the stability of the MAPbBr₃ single-crystal microwire arrays. Consequently, these MAPbBr₃ single-crystal microwire-array-based photodetectors exhibit significant long-term stability, maintaining 96% of the initial photocurrent after 1 year without further encapsulation. The lifetime of such photodetectors is hence approximately four times longer than that of the most stable previously reported perovskite micro/nanowire-based photodetector; this is thought to be the most stable perovskite photodetector reported thus far. Furthermore, this work should contribute further toward the realization of perovskite 1D structures with long-term stability.     

All-Oxide Transparent Photodetector Array for Ultrafast Response through Self-Powered Excitonic Photovoltage Operation

Can photodetectors be transparent and operate in self-powered mode? Is it possible to achieve invisible electronics, independent of the external power supply system, for on-site applications? Here, a ZnO/NiO heterojunction-based high-functional transparent ultraviolet (UV) photodetector operating in the self-powered photovoltaic mode with outstanding responsivity and detectivity values of 6.9 A W⁻¹ and 8.0 × 10¹² Jones, respectively, is reported. The highest I_UV/I_dark value of 8.9 × 10⁴ is attained at a wavelength of 385 nm, together with a very small dark current value of 9.15 × 10⁻¹² A. A large-scale sputtering method is adopted to deposit the heterostructure of n-ZnO and p-NiO sequentially. This deposition instinctively forms an abrupt junction, resulting in a high-quality heterojunction device. Moreover, developing a ZnO/NiO-heterojunction–based 4 × 5 matrix array with an output photovoltage of 4.5 V is preferred for integrating photodetectors into sensing and imaging systems. This transparent UV photodetector exhibits the fastest photo-response time (83 ns) reported for array configurations, which is achieved using an exciton-induced photovoltage based on a neutral donor–bound exciton. Overall, this study provides a simple method for achieving a high-performance large-scale transparent UV photodetector with a self-powered array configuration.     

Solution‐Processed 3D RGO–MoS2/Pyramid Si Heterojunction for Ultrahigh Detectivity and Ultra‐Broadband Photodetection

Molybdenum disulfide (MoS₂), a typical 2D metal dichalcogenide (2DMD), has exhibited tremendous potential in optoelectronic device applications, especially in photodetection. However, due to the weak light absorption of planar mono‐/multilayers, limited cutoff wavelength edge, and lack of high‐quality junctions, most reported MoS₂‐based photodetectors show undesirable performance. Here, a structurized 3D heterojunction of RGO–MoS₂/pyramid Si is demonstrated via a simple solution‐processing method. Owing to the improved light absorption by the pyramid structure, the narrowed bandgap of the MoS₂ by the imperfect crystallinity, and the enhanced charge separation/transportation by the inserted reduced graphene oxide (RGO), the assembled photodetector exhibits excellent performance in terms of a large responsivity of 21.8 A W^?1, extremely high detectivity up to 3.8 × 10¹⁵ Jones (Jones = cm Hz^1/2 W^?1) and ultrabroad spectrum response ranging from 350 nm (ultraviolet) to 4.3 µm (midwave infrared). These device parameters represent the best results for MoS₂‐based self‐driven photodetectors, and the detectivity value sets a new record for the 2DMD‐based photodetectors reported thus far. Prospectively, the design of novel 3D heterojunction can be extended to other 2DMDs, opening up the opportunities for a host of high‐performance optoelectronic devices.     

High-performance UV–vis photodetectors based on electrospun ZnO nanofiber-solution processed perovskite hybrid structures

Hybrid organic-inorganic perovskites have been demonstrated as promising candidates for broadband-responsive photodetectors.It is critical to develop perovskite-based photodetectors with excellent photodetection capability and facile fabrication processes for practical application.Herein,we designed and fabricated,for the first time,a hybrid photodetector consisting of electrospun ZnO nanofibers and perovskites.Compared to pristine ZnO or perovskite,the hybrid photodetector showed increased on-off ratio,faster response speed,and higher responsivity and detectivity.The performance of the hybrid devices was significantly enhanced by using quasi-aligned ZnO nanofiber arrays instead of disordered nanofibers,which provide efficient charge transfer between the perovskite and ZnO,shorter transmission paths,and reduced carrier loss at cross-junctions of nanofibers.Our results provide a new and promising route to integrate inorganic functional materials with perovskite for high-performance and low-cost photodetectors.     

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.     

Heterogeneous Integration of Carbon‐Nanotube–Graphene for High‐Performance,Flexible, and Transparent Photodetectors

Low‐dimensional carbon materials, such as semiconducting carbon nanotubes (CNTs), conducting graphene, and their hybrids, are of great interest as promising candidates for flexible, foldable, and transparent electronics. However, the development of highly photoresponsive, flexible, and transparent optoelectronics still remains limited due to their low absorbance and fast recombination rate of photoexcited charges, despite the considerable potential of photodetectors for future wearable and foldable devices. This work demonstrates a heterogeneous, all‐carbon photodetector composed of graphene electrodes and porphyrin‐interfaced single‐walled CNTs (SWNTs) channel, exhibiting high photoresponse, flexibility, and full transparency across the device. The porphyrin molecules generate and transfer photoexcited holes to the SWNTs even under weak white light, resulting in significant improvement of photoresponsivity from negligible to 1.6 × 10^?2 A W^?1. Simultaneously, the photodetector exhibits high flexibility allowing stable light detection under ≈50% strain (i.e., a bending radius of ≈350 µm), and retaining a sufficient transparency of ≈80% at 550 nm. Experimental demonstrations as a wearable sunlight sensor highlight the utility of the photodetector that can be conformally mounted on human skin and other curved surfaces without any mechanical and optical constraints. The heterogeneous integration of porphyrin–SWNT–graphene may provide a viable route to produce invisible, high‐performance optoelectronic systems.     

In Situ Formed Gradient Bandgap-Tunable Perovskite for Ultrahigh-Speed Color/Spectrum-Sensitive Photodetectors via Electron-Donor Control

Integration of various photodetectors with different light-sensitive materials and detection capacity is an inevitable way to achieve entire color/spectrum detection. However, the uneven capacity of each photodetector would drag the overall performance behind, especially the response speed. A response time down to nanosecond level has not previously been reported for a filter-free color/spectrum-sensitive photodetector, as far as is known. Here, a self-powered filterless color-sensitive photodetection array based on an in situ formed gradient perovskite absorber film with continuously tunable bandgap is demonstrated. Ultrahigh-speed response at nanosecond level is achieved in all the ingredient photodetectors. The junction capacitance being influenced by carrier concentration in the absorber is identified to be responsible for the detection speed. Without any optic or mechanical supporting system, the designed color detector exhibits an external quantum efficiency (EQE) up to 94% and a high spectral resolution of around 80 nm for the whole visible spectrum. This work offers a guidance to achieve fast response of perovskite-based photodetectors from the point of view of carrier-donor control and demonstrates a new avenue to establish color-sensitive photodetectors/spectrometers.