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.     

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.     

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.     

High‐Responsivity Photodetection by a Self‐Catalyzed Phase‐Pure p‐GaAs Nanowire

Defects are detrimental for optoelectronics devices, such as stacking faults can form carrier‐transportation barriers, and foreign impurities (Au) with deep‐energy levels can form carrier traps and nonradiative recombination centers. Here, self‐catalyzed p‐type GaAs nanowires (NWs) with a pure zinc blende (ZB) structure are first developed, and then a photodetector made from these NWs is fabricated. Due to the absence of stacking faults and suppression of large amount of defects with deep energy levels, the photodetector exhibits room‐temperature high photoresponsivity of 1.45 × 10⁵ A W^?1 and excellent specific detectivity (D*) up to 1.48 × 10¹⁴ Jones for a low‐intensity light signal of wavelength 632.8 nm, which outperforms previously reported NW‐based photodetectors. These results demonstrate these self‐catalyzed pure‐ZB GaAs NWs to be promising candidates for optoelectronics applications.     

Low‐Noise and Large‐Linear‐Dynamic‐Range Photodetectors Based on Hybrid‐Perovskite Thin‐Single‐Crystals

Organic–inorganic halide perovskites are promising photodetector materials due to their strong absorption, large carrier mobility, and easily tunable bandgap. Up to now, perovskite photodetectors are mainly based on polycrystalline thin films, which have some undesired properties such as large defective grain boundaries hindering the further improvement of the detector performance. Here, perovskite thin‐single‐crystal (TSC) photodetectors are fabricated with a vertical p–i–n structure. Due to the absence of grain‐boundaries, the trap densities of TSCs are 10–100 folds lower than that of polycrystalline thin films. The photodetectors based on CH₃NH₃PbBr₃ and CH₃NH₃PbI₃ TSCs show low noise of 1–2 fA Hz^?1/2, yielding a high specific detectivity of 1.5 × 10¹³ cm Hz^1/2 W^?1. The absence of grain boundaries reduces charge recombination and enables a linear response under strong light, superior to polycrystalline photodetectors. The CH₃NH₃PbBr₃ photodetectors show a linear response to green light from 0.35 pW cm^?2 to 2.1 W cm^?2, corresponding to a linear dynamic range of 256 dB.     

A Self‐Powered and Flexible Organometallic Halide Perovskite Photodetector with Very High Detectivity

Flexible and self‐powered photodetectors (PDs) are highly desirable for applications in image sensing, smart building, and optical communications. In this paper, a self‐powered and flexible PD based on the methylammonium lead iodide (CH₃NH₃PBI₃) perovskite is demonstrated. Such a self‐powered PD can operate even with irregular motion such as human finger tapping, which enables it to work without a bulky external power source. In addition, with high‐quality CH₃NH₃PBI₃ perovskite thin film fabricated with solvent engineering, the PD exhibits an impressive detectivity of 1.22 × 10¹³ Jones. In the self‐powered voltage detection mode, it achieves a large responsivity of up to 79.4 V mW^?1 cm^?2 and a voltage response of up to ≈90%. Moreover, as the PD is made of flexible and transparent polymer films, it can operate under bending and functions at 360 ° of illumination. As a result, the self‐powered, flexible, 360 ° omnidirectional perovskite PD, featuring high detectivity and responsivity along with real‐world sensing capability, suggests a new direction for next‐generation optical communications, sensing, and imaging applications.     

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.     

Atomic‐Layer Deposition‐Assisted Double‐Side Interfacial Engineering for High‐Performance Flexible and Stable CsPbBr3 Perovskite Photodetectors toward Visible Light Communication Applications

Self‐powered photodetectors (PDs) based on inorganic metal halide perovskites are regarded as promising alternatives for the next generation of photodetectors. However, uncontrollable film growth and sluggish charge extraction at interfaces directly limit the sensitivity and response speed of perovskite‐based photodetectors. Herein, by assistance of an atomic layer deposition (ALD) technique, CsPbBr₃ perovskite thin films with preferred orientation and enlarged grain size are obtained on predeposited interfacial modification layers. Thanks to improved film quality and double side interfacial engineering, the optimized CsPbBr₃ (Al₂O₃/CsPbBr₃/TiO₂, ACT) perovskite PDs exhibit outstanding performance with ultralow dark current of 10^?11 A, high detectivity of 1.88 × 10¹³ Jones and broad linear dynamic range (LDR) of 172.7 dB. Significantly, excellent long‐term environmental stability (ambient conditions >100 d) and flexibility stability (>3000 cycles) are also achieved. The remarkable performance is credited to the synergistic effects of high carrier conductivity and collection efficiency, which is assisted by ALD modification layers. Finally, the ACT PDs are successfully integrated into a visible light communication system as a light receiver on transmitting texts, showing a bit rate as high as 100 kbps. These results open the window of high performance all‐inorganic halide perovskite photodetectors and extends to rational applications for optical communication.     

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.     

Hydrogen Terminated Germanene for a Robust Self‐Powered Flexible Photoelectrochemical Photodetector

As a rising star in the family of graphene analogues, germanene shows great potential for electronic and optical device applications due to its unique structure and electronic properties. It is revealed that the hydrogen terminated germanene not only maintains a high carrier mobility similar to that of germanene, but also exhibits strong light–matter interaction with a direct band gap, exhibiting great potential for photoelectronics. In this work, few‐layer germanane (GeH) nanosheets with controllable thickness are successfully synthesized by a solution‐based exfoliation–centrifugation route. Instead of complicated microfabrication techniques, a robust photoelectrochemical (PEC)‐type photodetector, which can be extended to flexible device, is developed by simply using the GeH nanosheet film as an active electrode. The device exhibits an outstanding photocurrent density of 2.9 µA cm^?2 with zero bias potential, excellent responsivity at around 22 µA W^?1 under illumination with intensity ranging from 60 to 140 mW cm^?2, as well as short response time (with rise and decay times, t_r = 0.24 s and t_d = 0.74 s). This efficient strategy for a constructing GeH‐based PEC‐type photodetector suggests a path to promising high‐performance, self‐powered, flexible photodetectors, and it also paves the way to a practical application of germanene.     

Improving All‐Inorganic Perovskite Photodetectors by Preferred Orientation and Plasmonic Effect

All‐inorganic perovskites have high carrier mobility, long carrier diffusion length, excellent visible light absorption, and well overlapping with localized surface plasmon resonance (LSPR) of noble metal nanocrystals (NCs). The high‐performance photodetectors can be constructed by means of the intrinsic outstanding photoelectric properties, especially plasma coupling. Here, for the first time, inorganic perovskite photodetectors are demonstrated with synergetic effect of preferred‐orientation film and plasmonic with both high performance and solution process virtues, evidenced by 238% plasmonic enhancement factor and 10⁶ on/off ratio. The CsPbBr₃ and Au NC inks are assembled into high‐quality films by centrifugal‐casting and spin‐coating, respectively, which lead to the low cost and solution‐processed photodetectors. The remarkable near‐field enhancement effect induced by the coupling between Au LSPR and CsPbBr₃ photogenerated carriers is revealed by finite‐difference time‐domain simulations. The photodetector exhibits a light on/off ratio of more than 10⁶ under 532 nm laser illumination of 4.65 mW cm^?2. The photocurrent increases from 0.67 to 2.77 μA with centrifugal‐casting. Moreover, the photocurrent rises from 245.6 to 831.1 μA with Au NCs plasma enhancement, leading to an enhancement factor of 238%, which is the most optimal report among the LSPR‐enhanced photodetectors, to the best of our knowledge. The results of this study suggest that all‐inorganic perovskites are promising semiconductors for high‐performance solution‐processed photodetectors, which can be further enhanced by Au plasmonic effect, and hence have huge potentials in optical communication, safety monitoring, and biological sensing.     

Nested Inverse Opal Perovskite toward Superior Flexible and Self-Powered Photodetection Performance

Flexible and self-powered perovskite photodetectors have attracted tremendous research interests due to their applications in wearable and portable devices. However, the conventional planar structured photodetectors are always accompanied with limited device performance and undesired mechanical stability. Herein, a nested inverse opal (NIO) structured perovskite photodetector via a facile template-assisted spin-coating method is reported. The coupling effect of enhanced light capture, increased carrier transport, and improved perovskite film quality enables NIO device to exhibit superior photoresponse performance. The NIO photodetector exhibits a high responsivity of 473 mA W⁻¹ and detectivity up to 1.35 × 10¹³ Jones at 720 nm without external bias. The NIO structure can efficiently release mechanical stress during the bending process and the photocurrent has no degradation even after 500 cycles of bending. Moreover, the unencapsulated NIO device can operate for over 16 d under ambient conditions, presenting a significantly enhanced environmental stability compared to the planar device. This work demonstrates that deliberate structural design is an effective avenue for constructing self-powered, flexible, and stable optoelectronic devices.     

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.     

High‐Gain 200 ns Photodetectors from Self‐Aligned CdS–CdSe Core–Shell Nanowalls

1D core–shell heterojunction nanostructures have great potential for high‐performance, compact optoelectronic devices owing to their high interface area to volume ratio, yet their bottom‐up assembly toward scalable fabrication remains a challenge. Here the site‐controlled growth of aligned CdS–CdSe core–shell nanowalls is reported by a combination of surface‐guided vapor–liquid–solid horizontal growth and selective‐area vapor–solid epitaxial growth, and their integration into photodetectors at wafer‐scale without postgrowth transfer, alignment, or selective shell‐etching steps. The photocurrent response of these nanowalls is reduced to 200 ns with a gain of up to 3.8 × 10³ and a photoresponsivity of 1.2 × 10³ A W^?1, the fastest response at such a high gain ever reported for photodetectors based on compound semiconductor nanostructures. The simultaneous achievement of sub‐microsecond response and high‐gain photocurrent is attributed to the virtues of both the epitaxial CdS–CdSe heterojunction and the enhanced charge‐separation efficiency of the core–shell nanowall geometry. Surface‐guided nanostructures are promising templates for wafer‐scale fabrication of self‐aligned core–shell nanostructures toward scalable fabrication of high‐performance compact photodetectors from the bottom‐up.     

Self‐Powered Si/CdS Flexible Photodetector with Broadband Response from 325 to 1550 nm Based on Pyro‐phototronic Effect: An Approach for Photosensing below Bandgap Energy

Cadmium sulfide (CdS) has received widespread attention as the building block of optoelectronic devices due to its extraordinary optoelectronic properties, low work function, and excellent thermal and chemical stability. Here, a self‐powered flexible photodetector (PD) based on p‐Si/n‐CdS nanowires heterostructure is fabricated. By introducing the pyro‐phototronic effect derived from wurtzite structured CdS, the self‐powered PD shows a broadband response range, even beyond the bandgap limitation, from UV (325 nm) to near infrared (1550 nm) under zero bias with fast response speed. The light‐induced pyroelectric potential is utilized to modulate the optoelectronic processes and thus improve the photoresponse performance. Lasers with different wavelengths have different effects on the self‐powered PDs and corresponding working mechanisms are carefully investigated. Upon 325 nm laser illumination, the rise time and fall time of the self‐powered PD are 245 and 277 µs, respectively, which are faster than those of most previously reported CdS‐based nanostructure PDs. Meanwhile, the photoresponsivity R and specific detectivity D* regarding to the relative peak‐to‐peak current are both enhanced by 67.8 times, compared with those only based on the photovoltaic effect‐induced photocurrent. The self‐powered flexible PD with fast speed, stable, and broadband response is expected to have extensive applications in various environments.     

High‐Performance Photoelectrochemical‐Type Self‐Powered UV Photodetector Using Epitaxial TiO2/SnO2 Branched Heterojunction Nanostructure

TiO₂/SnO₂ branched heterojunction nanostructure with TiO₂ branches on electrospun SnO₂ nanofiber (B‐SnO₂ NF) networks serves as a model architecture for efficient self‐powered UV photodetector based on a photoelectrochemical cell (PECC). The nanostructure simultaneously offers a low degree of charge recombination and a direct pathway for electron transport. Without correcting 64.5% loss of incident photons through light absorption and scattering by the F‐doped tin oxide (FTO) glass, the incident power conversion efficiency reaches 14.7% at 330 nm, more than twice as large as the nanocrystalline TiO₂ (TiO₂ NC, 6.4%)‐film based PECC. By connecting a PECC to an ammeter, the intensity of UV light is quantified using the output short‐circuit photocurrent density (J_sc) without a power source. Under UV irradiation, the self‐powered UV photodetector exhibits a high responsivity of 0.6 A/W, a high on/off ratio of 4550, a rise time of 0.03 s and a decay time of 0.01 s for J_sc signal. The excellent performance of the B‐SnO₂ NF‐based PECC type self‐powered photodetector will enable significant advancements for next‐generation photodetection and photosensing applications.     

Epitaxial Growth of Large‐Grain NiSe Films by Solid‐State Reaction for High‐Responsivity Photodetector Arrays

Film‐based photodetectors have shown superiority for the fabrication of photodetector arrays, which are desired for integrating photodetectors into sensing and imaging systems, such as image sensors. But they usually possess a low responsivity due to low carrier mobility of the film consisting of nanocrystals. Large‐grain semiconductor films are expected to fabricate superior‐responsivity photodetector arrays. However, the growth of large‐grain semiconductor films, normally with a nonlayer structure, is still challenging. Herein, this study introduces a solid‐state reaction method, in which the growth rate is supposed to be limited by diffusion and reaction rate, for interface‐confined epitaxial growth of nonlayer structured NiSe films with grain size up to micrometer scale on Ni foil. Meanwhile, patterned growth of NiSe films allows the fabrication of NiSe film based photodetector arrays. More importantly, the fabricated photodetector based on as‐grown high‐quality NiSe films shows a responsivity of 150 A W^?1 in contrast to the value of 0.009 A W^?1 from the photodetector based on as‐deposited NiSe film consisting of nanocrystals, indicating a huge responsivity‐enhancement up to four orders of magnitude. It is ascribed to the enhanced charge carrier mobility in as‐grown NiSe films by dramatically decreasing the amount of grain boundary leading to scattering of charge carrier.     

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.     

Gate‐Controlled Graphene–Silicon Schottky Junction Photodetector

Various photodetectors showing extremely high photoresponsivity have been frequently reported, but many of these photodetectors could not avoid the simultaneous amplification of dark current. A gate‐controlled graphene–silicon Schottky junction photodetector that exhibits a high on/off photoswitching ratio (≈10⁴), a very high photoresponsivity (≈70 A W⁻¹), and a low dark current in the order of µA cm⁻² in a wide wavelength range (395–850 nm) is demonstrated. The photoresponsivity is ≈100 times higher than that of existing commercial photodetectors, and 7000 times higher than that of graphene‐field‐effect transistor‐based photodetectors, while the dark current is similar to or lower than that of commercial photodetectors. This result can be explained by a unique gain mechanism originating from the difference in carrier transport characteristics of silicon and graphene.     

Phase‐Engineered Type‐II Multimetal–Selenide Heterostructures toward Low‐Power Consumption,Flexible, Transparent,and Wide‐Spectrum Photoresponse Photodetectors

Phase‐engineered type‐II metal–selenide heterostructures are demonstrated by directly selenizing indium‐tin oxide to form multimetal selenides in a single step. The utilization of a plasma system to assist the selenization facilitates a low‐temperature process, which results in large‐area films with high uniformity. Compared to single‐metal–selenide‐based photodetectors, the multimetal–selenide photodetectors exhibit obviously improved performance, which can be attributed to the Schottky contact at the interface for tuning the carrier transport, as well as the type‐II heterostructure that is beneficial for the separation of the electron–hole pairs. The multimetal–selenide photodetectors exhibit a response to light over a broad spectrum from UV to visible light with a high responsivity of 0.8 A W^?1 and an on/off current ratio of up to 10². Interestingly, all‐transparent photodetectors are successfully produced in this work. Moreover, the possibility of fabricating devices on flexible substrates is also demonstrated with sustainable performance, high strain tolerance, and high durability during bending tests.