Broadband Photoresponse Enhancement of a High‐Performance t‐Se Microtube Photodetector by Plasmonic Metallic Nanoparticles

Broadband responsivity enhancement of single Se microtube (Se‐MT) photodetectors in the UV–visible region is presented in this research. The pristine Se‐MT photodetector demonstrates broadband photoresponse from 300 to 700 nm with peak responsivity of ≈19 mA W^?1 at 610 nm and fast speed (rise time 0.32 ms and fall time 23.02 ms). To further enhance the responsivity of the single Se‐MT photodetector, Au and Pt nanoparticles (NPs) are sputtered on these devices. In contrast to only enhancement of responsivity in UV region by Pt NPs, broadband responsivity enhancement (≈600% to ≈800%) of the Se‐MT photodetector is realized from 300 to 700 nm by tuning the size and density of Au NPs. The broadband responsivity enhancement phenomena are interpreted by both the surface modification and surface plasmon coupling. The experimental results of this work provide an additional opportunity for fabricating high‐performance UV–visible broadband photodetectors.     

An Ultrahigh Responsivity (9.7 mA W−1) Self‐Powered Solar‐Blind Photodetector Based on Individual ZnO–Ga2O3 Heterostructures

Highly crystallized ZnO–Ga₂O₃ core–shell heterostructure microwire is synthesized by a simple one‐step chemical vapor deposition method, and constructed into a self‐powered solar‐blind (200–280 nm) photodetector with a sharp cutoff wavelength at 266 nm. The device shows an ultrahigh responsivity (9.7 mA W^?1) at 251 nm with a high UV/visible rejection ratio (R _{251 nm}/R _{400 nm}) of 6.9 × 10² under zero bias. The self‐powered device has a fast response speed with rise time shorter than 100 µs and decay time of 900 µs, respectively. The ultrahigh responsivity, high UV/visible rejection ratio, and fast response speed make it highly suitable in practical self‐powered solar‐blind detection. Additinoally, this microstructure heterojunction design method would provide a new approach to realize the high‐performance self‐powered photodetectors.     

Flexible and Self‐Powered Lateral Photodetector Based on Inorganic Perovskite CsPbI3–CsPbBr3 Heterojunction Nanowire Array

Self‐powered perovskite photodetectors mainly adopt the vertical heterojunction structure composed of active layer, electron–hole transfer layers, and electrodes, which results in the loss of incident light and interfacial accumulation of defects. To address these issues, a self‐powered lateral photodetector based on CsPbI₃–CsPbBr₃ heterojunction nanowire arrays is designed on both a rigid glass and a flexible polyethylene naphthalate substrate using an in situ conversion and mask‐assisted electrode fabrication method. Through adding the polyvinyl pyrrolidone and optimizing the concentration of precursors under the pressure‐assisted moulding process, both the crystallinity and stability of perovskite nanowire array are improved. The nanowire array–based lateral device shows a high responsivity of 125 mA W^?1 and a fast rise and decay time of 0.7 and 0.8 ms under a self‐powered operation condition. This work provides a new strategy to fabricate perovskite heterojunction nanoarrays towards self‐powered photodetection.     

Response Enhancement of Self‐Powered Visible‐Blind UV Photodetectors by Nanostructured Heterointerface Engineering

The development of efficient photodetectors (PDs) for ultraviolet (UV) light is of great importance for many applications. In this paper, a novel approach is proposed for boosting the performances of self‐powered PDs. Visible‐blind UV‐A PDs are built by combining a mesoporous TiO₂ layer with a Spiro‐OMeTAD layer. The nanostructured heterointerface is engineered by inserting a self‐assembled layer of organic modifiers. By choosing 4‐nitrobenzoic acid (NBA), the responsivity is boosted by 70% compared to the pristine devices. It achieves 64 mA W^?1 at 0 V bias, 380 nm, and 1 mW cm^?2. The PD displays a very high sensitivity (>10⁴), a fast response time (<3 ms), a high stability, and repeatability. 4‐chlorobenzoic acid, 4‐methoxy benzoic acid, 4‐nitro benzoic acid, and β‐alanine surface modifiers are studied by a combined experimental and theoretical approach. Their dipole moment is calculated. Their presence induces a step in the vacuum energy and the formed dipole field dramatically affects the charge transfer and then the photocurrent/photoresponse of the device. The higher responsivity of the NBA‐modified PD is thus explained by the better and faster electron charge transfer toward the electrical contact on TiO₂.     

Ultrasensitive Room‐Temperature Terahertz Direct Detection Based on a Bismuth Selenide Topological Insulator

Despite their huge application capabilities, millimeter‐ and terahertz‐wave photodetectors still face challenges in the detection scheme. Topological insulators (TIs) are predicted to be promising candidates for long‐wavelength photodetection, due to the presence of Dirac fermions in their topologically protected surface states. However, photodetection based on TIs is usually hindered by the large dark current, originating from the mixing of bulk states with topological surface states (TSSs) in most realistic samples of TIs. Here millimeter and terahertz detectors based on a subwavelength metal–TI–metal (MTM) heterostructure are demonstrated. The achieved photoresponse stems from the asymmetric scattering of TSS, driven by the localized surface plasmon‐induced terahertz field, which ultimately produces direct photocarriers beyond the interband limit. The device enables high responsivity in both the self‐powered and bias modes even at room temperature. The achieved responsivity is over 75 A/W, with response time shorter than 60 ms in the self‐powered mode. Remarkably, the responsivity increases by several orders of magnitude in the biased configuration, with the noise‐equivalent power (NEP) of 3.6 × 10^?13 W Hz^?1/2 and a detectivity of 2.17 × 10¹¹ cm Hz^?1/2 W^?1 at room temperature. The detection performances open a way toward realistic exploitation of TIs for large‐area, real‐time imaging within long‐wavelength optoelectronics.     

Structural Design and Pyroelectric Property of SnS/CdS Heterojunctions Contrived for Low‐Temperature Visible Photodetectors

The traditional photodetectors based on photoelectric effect exhibit inferior response or even out of operation with the decrease of temperature. However, cryogenic visible light detection is increasingly demanded in deep space and polar exploration. Herein, a self‐powered visible photodetector coupling pyroelectricity and photoelectricity to optimize the cryogenic detecting performance is designed in which hydrothermally grown CdS nanorod array is covered by SnS nanoflakes. The choice of SnS allows the detector with strong visible light absorption and great photoelectric conversion efficiency, while the CdS nanorod structure with pyroelectricity can effectively modulate the behavior of photogenerated carriers at low temperatures. It is found that the response characteristics of the photodetector are dominated by the combination of pyroelectric and photoelectric effects, which becomes more significant with the reduced temperature. Specifically, at 130 K temperature, the photoresponse current under 650 nm light is improved by 7.5 times as that at room temperature, while the ratio of pyroelectric current to photocurrent can be increased to 400%. Meanwhile, the responsivity and detectivity are as high as 10.4 mA W^?1 and 3.56 × 10¹¹ Jones, respectively. This work provides a promising approach to develop high‐performance self‐powered visible photodetectors with low‐temperature operating capability.     

Comprehensive Pyro‐Phototronic Effect Enhanced Ultraviolet Detector with ZnO/Ag Schottky Junction

As a coupling effect of pyroelectric and photoelectric effect, pyro‐phototronic effect has demonstrated an excellent tuning role for fast response p–n junction photodetectors (PDs). Here, a comprehensive pyro‐phototronic effect is utilized to design and fabricate a self‐powered and flexible ultraviolet PD based on the ZnO/Ag Schottky junction. By using the primary pyroelectric effect, the maximal transient photoresponsivity of the self‐powered PDs can reach up to 1.25 mA W^?1 for 325 nm illumination, which is improved by 1465% relative to that obtained from the steady‐state signal. The relative persistent secondary pyroelectric effect weakens the height of Schottky barrier, leading to a reduction of the steady‐state photocurrent with an increase in the power density. When the power density is large enough, the steady‐state photocurrent turns into a reverse direction. The corresponding tuning mechanisms of the comprehensive pyro‐phototronic effect on transient and steady‐state photocurrent are revealed based on the bandgap diagrams. The results may help us to further clarify the mechanism of the pyro‐phototronic effect on the photocurrent and also provide a potential way to optimize the performance of self‐powered PDs.     

Triboelectric Nanogenerator as an Active UV Photodetector

Self‐powered nanosensors and nanosystems have attracted significant attention in the past decades and have gradually become the most desirable and promising prototype for environmental protection/detection because no battery is needed to power the device. Therefore, in this paper a design is proposed for a self‐powered photodetector based on triboelectric nanogenerator (TENG) configuration. 3D dendritic TiO₂ nanostructures are synthesized as the built‐in UV photodetector as well as the contact material of the TENG. The cost‐effective, robust, and easily fabricated TENG‐based photodetector presents superior photoresponse characteristics, which include an excellent responsivity over 280 A W^?1, rapid rise time (18 ms) and decay time (31 ms), and a wide detection range of light intensity from 20 μW cm^?2 to 7 mW cm^?2. In the last part of the paper, a stand‐alone and self‐powered environmental sensing device is developed by applying poly(methyl methacrylate) (PMMA) substrates and springs to assemble the TENG‐based photodetector. These results indicate that the new prototype sensing device based on the TENG configuration shows great potential as a self‐powered photodetector.     

Large‐Size Growth of Ultrathin SnS2 Nanosheets and High Performance for Phototransistors

2D SnS₂ nanosheets have been attracting intensive attention as one potential candidate for the modern electronic and/or optoelectronic fields. However, the controllable large‐size growth of ultrathin SnS₂ nanosheets still remains a great challenge and the photodetectors based on SnS₂ nanosheets suffer from low responsivity, thus hindering their further applications so far. Herein, an improved chemical vapor deposition route is provided to synthesize large‐size SnS₂ nanosheets, the side length of which can surpass 150 μm. Then, ultrathin SnS₂ nanosheet‐based phototransistors are fabricated, which achieve high photoresponsivities up to 261 A W^?1 (with a fast rising time of 20 ms and a falling time of 16 ms) in air and 722 A W^?1 in vacuum, respectively. Furthermore, the effects of back‐gate voltage and air adsorbates on the optoelectronic properties of the SnS₂ nanosheet have been systematically investigated. In addition, a high‐performance flexible photodetector based on SnS₂ nanosheet is also fabricated with a high responsivity of 34.6 A W^?1.     

High‐Performance All‐Polymer Photoresponse Devices Based on Acceptor–Acceptor Conjugated Polymers

Three acceptor–acceptor (A–A) type conjugated polymers based on isoindigo and naphthalene diimide/perylene diimide are designed and synthesized to study the effects of building blocks and alkyl chains on the polymer properties and performance of all‐polymer photoresponse devices. Variation of the building blocks and alkyl chains can influence the thermal, optical, and electrochemical properties of the polymers, as indicated by thermogravimetric analysis, differential scanning calorimetry, UV–vis, cyclic voltammetry, and density functional theory calculations. Based on the A–A type conjugated polymers, the most efficient all‐polymer photovoltaic cells are achieved with an efficiency of 2.68%, and the first all‐polymer photodetectors are constructed with high responsivity (0.12 A W^?1) and detectivity (1.2 × 10¹² Jones), comparable to those of the best fullerene based organic photodetectors and inorganic photodetectors. Photoluminescence spectra, charge transport properties, and morphology of blend films are investigated to elucidate the influence of polymeric structures on device performances. This contribution demonstrates a strategy of systematically tuning the polymeric structures to achieve high performance all‐polymer photoresponse devices.     

Mixed‐Valence‐Driven Quasi‐1D SnIISnIVS3 with Highly Polarization‐Sensitive UV–vis–NIR Photoresponse

Mixed‐valence states can bring unexpected unique phenomena, especially novel anisotropic physics, due to structural asymmetry, which originate from the discrepant distribution of atoms with different valence. This study reports an unexploited mixed‐valence‐driven quasi‐1D Sn^IISn^IVS₃ crystal, which exhibits widely and distinctively anisotropic polarized‐light absorption reaching ≈3.4 from the deep ultraviolet to near‐infrared region (250–850 nm). The fabricated polarization‐sensitive photodetectors based on highly air‐stable Sn^IISn^IVS₃ nanowires display strong linear dichroism among the UV–vis–NIR spectrum with responsivity exceeding ≈150 A W^?1. Furthermore, the devices are further constructed onto a flexible polyethylene terephthalate (PET) substrate and the photoresponse remains roughly unchanged after repeated bending. This work based on novel mixed‐valence‐driven quasi‐1D ternary sulfide Sn^IISn^IVS₃ excites interest in low‐symmetry semiconductors for developing broadly spectral polarization‐sensitive photodetectors with environmental stability and mechanical flexibility.     

High—Performance Solar‐Blind Deep Ultraviolet Photodetector Based on Individual Single‐Crystalline Zn2GeO4 Nanowire

Solar‐blind deep ultraviolet (DUV) photodetectors have been a hot topic in recent years because of their wide commercial and military applications. A wide bandgap (4.68 eV) of ternary oxide Zn₂GeO₄ makes it an ideal material for the solar‐blind DUV detection. Unfortunately, the sensing performance of previously reported photodetectors based on Zn₂GeO₄ nanowires has been unsatisfactory for practical applications, because they suffer from long response and decay times, low responsivity, and quantum efficiency. Here, high‐performance solar‐blind DUV photodetectors are developed based on individual single‐crystalline Zn₂GeO₄ nanowires. The transport mechanism is discussed in the frame of the small polaron theory. In situ electrical characterization of individual Zn₂GeO₄ nanowires reveals a high gain under high energy electron beam. The devices demonstrate outstanding solar‐blind light sensing performances: a responsivity of 5.11 × 10³ A W^?1, external quantum efficiency of 2.45 × 10⁶%, detectivity of ≈2.91 × 10¹¹ Jones, τ_rise ≈ 10 ms, and τ_decay ≈ 13 ms, which are superior to all reported Zn₂GeO₄ and other ternary oxide nanowire photodetectors. These results render the Zn₂GeO₄ nanowires particularly valuable for optoelectronic devices.     

High‐Performance UV–Vis–NIR Phototransistors Based on Single‐Crystalline Organic Semiconductor–Gold Hybrid Nanomaterials

Hybrid materials in optoelectronic devices can generate new functionality or provide synergistic effects that enhance the properties of each component. Here, high‐performance phototransistors with broad spectral responsivity in UV–vis–near‐infrared (NIR) regions, using gold nanorods (Au NRs)‐decorated n‐type organic semiconductor and N ,N ′‐bis(2‐phenylethyl)‐perylene‐3,4:9,10‐tetracarboxylic diimide (BPE‐PTCDI) nanowires (NWs) are reported. By way of the synergistic effect of the excellent photo‐conducting characteristics of single‐crystalline BPE‐PTCDI NW and the light scattering and localized surface plasmon resonances (LSPR) of Au NRs, the hybrid system provides new photo‐detectivity in the NIR spectral region. In the UV–vis region, hybrid nanomaterial‐based phototransistors exhibit significantly enhanced photo‐responsive properties with a photo‐responsivity (R ) of 7.70 × 10⁵ A W^?1 and external quantum efficiency (EQE) of 1.42 × 10⁸% at the minimum light intensity of 2.5 µW cm^?2, which are at least tenfold greater than those of pristine BPE‐PTCDI NW‐based ones and comparable to those of high‐performance inorganic material‐based devices. While a pristine BPE‐PTCDI NW‐based photodetector is insensitive to the NIR spectral region, the hybrid NW‐based phototransistor shows an R of 10.7 A W^?1 and EQE of 1.35 × 10³% under 980 nm wavelength‐NIR illumination. This work demonstrates a viable approach to high‐performance photo‐detecting systems with broad spectral responsivity.     

Fine Control of Perovskite Crystallization and Reducing Luminescence Quenching Using Self‐Doped Polyaniline Hole Injection Layer for Efficient Perovskite Light‐Emitting Diodes

Organic–inorganic hybrid perovskites (OHPs) are promising emitters for light‐emitting diodes (LEDs) due to the high color purity, low cost, and simple synthesis. However, the electroluminescent efficiency of polycrystalline OHP LEDs (PeLEDs) is often limited by poor surface morphology, small exciton binding energy, and long exciton diffusion length of large‐grain OHP films caused by uncontrolled crystallization. Here, crystallization of methylammonium lead bromide (MAPbBr₃) is finely controlled by using a polar solvent‐soluble self‐doped conducting polymer, poly(styrenesulfonate)‐grafted polyaniline (PSS‐g‐PANI), as a hole injection layer (HIL) to induce granular structure, which makes charge carriers spatially confined more effectively than columnar structure induced by the conventional poly(3,4‐ethylenedioythiphene):polystyrenesulfonate (PEDOT:PSS). Moreover, lower acidity of PSS‐g‐PANI than PEDOT:PSS reduces indium tin oxide (ITO) etching, which releases metallic In species that cause exciton quenching. Finally, doubled device efficiency of 14.3 cd A^‐1 is achieved for PSS‐g‐PANI‐based polycrystalline MAPbBr₃ PeLEDs compared to that for PEDOT:PSS‐based PeLEDs (7.07 cd A^‐1). Furthermore, PSS‐g‐PANI demonstrates high efficiency of 37.6 cd A^‐1 in formamidinium lead bromide nanoparticle LEDs. The results provide an avenue to both control the crystallization kinetics and reduce the migration of In released from ITO by forming OIP films favorable for more radiative luminescence using the polar solvent‐soluble and low‐acidity polymeric HIL.     

Solution‐Processed Flexible Broadband Photodetectors with Solution‐Processed Transparent Polymeric Electrode

Room‐temperature solution‐processed flexible photodetectors with spectral response from 300 to 2600 nm are reported. Solution‐processed polymeric thin film with transparency ranging from 300 to 7000 nm and superior electrical conductivity as the transparent electrode is reported. Solution‐processed flexible broadband photodetectors with a “vertical” device structure incorporating a perovskite/PbSe quantum dot bilayer thin film based on the above solution‐processed transparent polymeric electrode are demonstrated. The utilization of perovskite/PbSe quantum dot bilayer thin film as the photoactive layer extends spectral response to infrared region and boosts photocurrent densities in both visible and infrared regions through the trap‐assisted photomultiplication effect. Operated at room temperature and under an external bias of ‐1 V, the solution‐processed flexible photodetectors exhibit over 230 mA W^‐1 responsivity, over 1011 cm Hz1/2/W photodetectivity from 300 to 2600 nm and ≈70 dB linear dynamic ranges. It is also found that the solution‐processed flexible broadband photodetectors exhibit fast response time and excellent flexibility. All these results demonstrate that this work develop a facile approach to realize room‐temperature operated ultrasensitive solution‐processed flexible broadband photodetectors with “vertical” device structure through solution‐processed transparent polymeric electrode.     

Self‐Powered Flexible TiO2 Fibrous Photodetectors: Heterojunction with P3HT and Boosted Responsivity and Selectivity by Au Nanoparticles

A novel inorganic–organic heterojunction (TiO₂/P3HT (poly(3‐hexylthiophene)) is easily prepared by a combination of anodization and vacuumed dip‐coating methods, and the constructed flexible fibrous photodetector (FPD) exhibits high‐performance self‐powered UV–visible broadband photoresponse with fast speed, high responsivity, and good stability, as well as highly stable performance at bending states, showing great potential for wearable electronic devices. Moreover, Au nanoparticles are deposited to further boost the responsivity and selectivity by regulating the sputtering intervals. The optimal Au/TiO₂/P3HT FPD yields an ≈700% responsivity enhancement at 0 V under 350 nm illumination. The sharp cut‐off edge and high UV–visible rejection ratio (≈17 times higher) indicate a self‐powered flexible UV photodetector. This work provides an effective and versatile route to modulate the photoelectric performance of flexible electronic devices.     

Ultrahigh‐Performance Flexible and Self‐Powered Photodetectors with Ferroelectric P(VDF‐TrFE)/Perovskite Bulk Heterojunction

Flexible and self‐powered perovskite photodetectors attract widespread research interests due to their potential applications in portable and wearable optoelectronic devices. However, the reported devices mainly adopt an independent layered structure with complex fabrication processes and high carrier recombination. Herein, an integrated ferroelectric poly(vinylidene‐fluoride‐trifluoroethylene) (P(VDF‐TrFE)) and perovskite bulk heterojunction film photodetector on the polyethylene naphthalate substrate is demonstrated. Under the optimum treatment conditions (the polarization voltage and time, and the concentration of P(VDF‐TrFE)), the photodetector exhibits a largely enhanced performance compared to the pristine perovskite device. The resulting device exhibits ultrahigh performance with a large detectivity (1.4 × 10¹³ Jones) and fast response time (92/193 µs) at the wavelength of 650 nm. The improved performance is attributed to the fact that the polarized P(VDF‐TrFE)/perovskite hybrid film provides a stronger built‐in electric field to facilitate the separation and transportation of photogenerated carriers. These findings provide a new route to design self‐powered photodetectors from the aspect of device structure and carrier transport.     

High‐Performance Near‐Infrared Photodetector Based on Ultrathin Bi2O2Se Nanosheets

As an emerging 2D layered material, Bi₂O₂Se has shown great potential for applications in thermoelectric and electronics, due to its high carrier mobility, near‐ideal subthreshold swing, and high air‐stability. Although Bi₂O₂Se has a suitable band gap for infrared (IR) applications, its photoresponse properties have not been investigated. Here, high‐quality ultrathin Bi₂O₂Se sheets are synthesized via a low‐pressure chemical vapor deposition method. The thickness of 90% Bi₂O₂Se sheets is below 10 nm and lateral sizes mainly distribute in the range of 7–11 µm. In addition, it is found that triangular sheets largely lack “O” content, even only 0.2 for Bi₂O_0.2Se. The near‐IR photodetection performance of Bi₂O₂Se nanosheets is systematically studied by variable temperature measurements. The response time, responsivity, and detectivity can approach up to 2.8 ms, 6.5 A W^?1, and 8.3 × 10¹¹ Jones, respectively. Additionally, the critical performance parameters, including responsivity, rising time, and decay time, remain at almost the same level when the temperature is changed from 80 to 300 K. These phenomena are likely due to the fact that as‐grown ultrathin Bi₂O₂Se sheets have no surface trap states and shallow defect energy levels. The findings indicate ultrathin Bi₂O₂Se sheets have great potentials for future applications in ultrafast, flexible near‐IR optoelectronic devices.     

Working Principles of Perovskite Photodetectors: Analyzing the Interplay Between Photoconductivity and Voltage‐Driven Energy‐Level Alignment

Organic–inorganic lead halide perovskites have recently received significant attention as active materials for high‐performance photovoltaics and photodetectors. However, the understanding of their operation mechanism remains limited. High‐gain, low‐voltage CH₃NH₃PbI₃ photodetectors in various architectures are demonstrated herein. Photomultiplication in all structures with direct contact of fluorine‐doped tin oxide (FTO) and perovskite with the highest responsivity 208 A W^?1 corresponding to an incident photon‐to‐current efficiency of 47 000% is observed. Studying the dynamics and temperature dependence, a slow process with an activation energy of 420 ± 90 meV in the time scale of seconds is found, which is essential to photocurrent multiplication. A model based on ion migration to explain the observed transients and the photomultiplication is developed. The accumulation of negative ionic charge at the FTO/perovskite interface under reverse bias lowers the FTO work function allowing for direct hole injection into the perovskite valence band. Under illumination, the conductivity of perovskite is increased and the device behaves similar to a photoconductor.     

MoS2/HfO2/Silicon‐On‐Insulator Dual‐Photogating Transistor with Ambipolar Photoresponsivity for High‐Resolution Light Wavelength Detection

Photogating detectors based on 2D materials attract significant research interests. However, most of these photodetectors are only sensitive to the incident intensities and lack the ability to distinguish different wavelengths. Color imaging based on these detectors usually requires additional optical filter arrays to collect red, green, and blue (RGB) colors in different photodetectors to restore the true color of one pixel. In this study, an MoS₂/HfO₂/silicon‐on‐insulator field effect phototransistor with wavelength distinguishing ability is presented, where the photogating effect can be simultaneously formed in the top MoS₂ gate and bottom Si substrate gate. These two individual photogating effects can reduce and increase the read current in the middle 12 nm Si channel, respectively. Thus, by tuning the applied voltages on these two gates, the device can be used to obtain tunable ambipolar photoresponsivity from +7000 A W^?1 (Si bottom gate dominated) to 0 A W^?1 (balanced), and finally to ?8000 A W^?1 (MoS₂ gate dominated). In addition, the experimental results show that the corresponding top gate voltage to the zero responsivity (0 A W^?1) point can be positively shifted by the increasing of incident wavelength with high resolution up to 2 nm and is insensitive to the incident intensity.