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.     

Non‐volatile Ferroelectric Poly(vinylidene fluoride‐co‐trifluoroethylene) Memory Based on a Single‐Crystalline Tri‐isopropylsilylethynyl Pentacene Field‐Effect Transistor

A new type of nonvolatile ferroelectric poly(vinylidene fluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)) memory based on an organic thin‐film transistor (OTFT) with a single crystal of tri‐isopropylsilylethynyl pentacene (TIPS‐PEN) as the active layer is developed. A bottom‐gate OTFT is fabricated with a thin P(VDF‐TrFE) film gate insulator on which a one‐dimensional ribbon‐type TIPS‐PEN single crystal, grown via a solvent‐exchange method, is positioned between the Au source and drain electrodes. Post‐thermal treatment optimizes the interface between the flat, single‐crystalline ab plane of TIPS‐PEN and the polycrystalline P(VDF‐TrFE) surface with characteristic needle‐like crystalline lamellae. As a consequence, the memory device exhibits a substantially stable source–drain current modulation with an ON/OFF ratio hysteresis greater than 10³, which is superior to a ferroelectric P(VDF‐TrFE) OTFT that has a vacuum‐evaporated pentacene layer. Data retention longer than 5 × 10⁴ s is additionally achieved in ambient conditions by incorporating an interlayer between the gate electrode and P(VDF‐TrFE) thin film. The device is environmentally stable for more than 40 days without additional passivation. The deposition of a seed solution of TIPS‐PEN on the chemically micropatterned surface allows fabrication arrays of TIPS‐PEN single crystals that can be potentially useful for integrated arrays of ferroelectric polymeric TFT memory.     

Control of Current Hysteresis of Networked Single‐Walled Carbon Nanotube Transistors by a Ferroelectric Polymer Gate Insulator

Films made of 2D networks of single‐walled carbon nanotubes (SWNTs) are one of the most promising active‐channel materials for field‐effect transistors (FETs) and have a variety of flexible electronic applications, ranging from biological and chemical sensors to high‐speed switching devices. Challenges, however, still remain due to the current hysteresis of SWNT‐containing FETs, which has hindered further development. A new and robust method to control the current hysteresis of a SWNT‐network FET is presented, which involves the non‐volatile polarization of a ferroelectric poly(vinylidene fluoride‐trifluoroethylene) (P(VDF‐TrFE)) gate insulator. A top‐gate FET with a solution‐processed SWNT‐network exhibits significant suppression of the hysteresis when the gate‐voltage sweep is greater than the coercive field of the ferroelectric polymer layer (≈50 MV m^?1). These near‐hysteresis‐free characteristics are believed to be due to the characteristic hysteresis of the P(VDF‐TrFE), resulting from its non‐volatile polarization, which makes effective compensation for the current hysteresis of the SWNT‐network FETs. The onset voltage for hysteresis‐minimized operation is able to be tuned simply by controlling the thickness of the ferroelectric film, which opens the possibility of operating hysteresis‐free devices with gate voltages down to a few volts.     

All‐Polymer Bistable Resistive Memory Device Based on Nanoscale Phase‐Separated PCBM‐Ferroelectric Blends

All polymer nonvolatile bistable memory devices are fabricated from blends of ferroelectric poly(vinylidenefluoride–trifluoroethylene (P(VDF‐TrFE)) and n‐type semiconducting [6,6]‐phenyl‐C61‐butyric acid methyl ester (PCBM). The nanoscale phase separated films consist of PCBM domains that extend from bottom to top electrode, surrounded by a ferroelectric P(VDF‐TrFE) matrix. Highly conducting poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) polymer electrodes are used to engineer band offsets at the interfaces. The devices display resistive switching behavior due to modulation of this injection barrier. With careful optimization of the solvent and processing conditions, it is possible to spin cast very smooth blend films (R_rms ≈ 7.94 nm) and with good reproducibility. The devices exhibit high I_on/I_off ratios (≈3 × 10³), low read voltages (≈5 V), excellent dielectric response at high frequencies (?_r ≈ 8.3 at 1 MHz), and excellent retention characteristics up to 10 000 s.     

High‐Performance Top‐Gated Organic Field‐Effect Transistor Memory using Electrets for Monolithic Printed Flexible NAND Flash Memory

High‐performance top‐gated organic field‐effect transistor (OFET) memory devices using electrets and their applications to flexible printed organic NAND flash are reported. The OFETs based on an inkjet‐printed p‐type polymer semiconductor with efficiently chargeable dielectric poly(2‐vinylnaphthalene) (PVN) and high‐k blocking gate dielectric poly(vinylidenefluoride‐trifluoroethylene) (P(VDF‐TrFE)) shows excellent non‐volatile memory characteristics. The superior memory characteristics originate mainly from reversible charge trapping and detrapping in the PVN electret layer efficiently in low‐k/high‐k bilayered dielectrics. A strategy is devised for the successful development of monolithically inkjet‐printed flexible organic NAND flash memory through the proper selection of the polymer electrets (PVN or PS), where PVN/‐ and PS/P(VDF‐TrFE) devices are used as non‐volatile memory cells and ground‐ and bit‐line select transistors, respectively. Electrical simulations reveal that the flexible printed organic NAND flash can be possible to program, read, and erase all memory cells in the memory array repeatedly without affecting the non‐selected memory cells.     

High‐Performance Ferroelectric Memory Based on Phase‐Separated Films of Polymer Blends

High‐performance polymer memory is fabricated using blends of ferroelectric poly(vinylidene‐fluoride‐trifluoroethylene) (P(VDF‐TrFE)) and highly insulating poly(p‐phenylene oxide) (PPO). The blend films spontaneously phase separate into amorphous PPO nanospheres embedded in a semicrystalline P(VDF‐TrFE) matrix. Using low molecular weight PPO with high miscibility in a common solvent, i.e., methyl ethyl ketone, blend films are spin cast with extremely low roughness (R_rms ≈ 4.92 nm) and achieve nanoscale phase seperation (PPO domain size < 200 nm). These blend devices display highly improved ferroelectric and dielectric performance with low dielectric losses (<0.2 up to 1 MHz), enhanced thermal stability (up to ≈353 K), excellent fatigue endurance (80% retention after 10⁶ cycles at 1 KHz) and high dielectric breakdown fields (≈360 MV/m).     

High‐Performance Piezoelectric,Pyroelectric, and Triboelectric Nanogenerators Based on P(VDF‐TrFE) with Controlled Crystallinity and Dipole Alignment

Poly(vinylidenefluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)), as a ferroelectric polymer, offers great promise for energy harvesting for flexible and wearable applications. Here, this paper shows that the choice of solvent used to dissolve the polymer significantly influences its properties in terms of energy harvesting. Indeed, the P(VDF‐TrFE) prepared using a high dipole moment solvent has higher piezoelectric and pyroelectric coefficients and triboelectric property. Such improvements are the result of higher crystallinity and better dipole alignment of the polymer prepared using a higher dipole moment solvent. Finite element method simulations confirm that the higher dipole moment results in higher piezoelectric, pyroelectric, and triboelectric potential distributions. Furthermore, P(VDF‐TrFE)‐based piezoelectric, pyroelectric, and triboelectric nanogenerators (NGs) experimentally validate that the higher dipole moment solvent significantly enhances the power output performance of the NGs; the improvement is about 24% and 82% in output voltage and current, respectively, for piezoelectric NG; about 40% and 35% in output voltage and current, respectively, for pyroelectric NG; and about 65% and 75% in output voltage and current for triboelectric NG. In brief, the approach of using a high dipole moment solvent is very promising for high output P(VDF‐TrFE)‐based wearable NGs.     

Micropatterned P(VDF‐TrFE) Film‐Based Piezoelectric Nanogenerators for Highly Sensitive Self‐Powered Pressure Sensors

Here micropatterned poly(vinylidenefluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)) films‐based piezoelectric nanogenerators (PNGs) with high power‐generating performance for highly sensitive self‐powered pressure sensors are demonstrated. The microstructured P(VDF‐TrFE)‐based PNGs reveal nearly five times larger power output compared to a flat film‐based PNG. The micropatterning of P(VDF‐TrFE) polymer makes itself ultrasensitive in response to mechanical deformation. The application is demonstrated successfully as self‐powered pressure sensors in which mechanical energy comes from water droplet and wind. The mechanism of the high performance is intensively discussed and illustrated in terms of strain developed in the flat and micropatterned P(VDF‐TrFE) films. The impact derived from the patterning on the output performance is studied in term of effective pressure using COMSOL multiphysics software.     

Electrode Dependence of Tunneling Electroresistance and Switching Stability in Organic Ferroelectric P(VDF‐TrFE)‐Based Tunnel Junctions

Ferroelectric tunnel junctions (FTJs) are promising candidates for nonvolatile memories and memristor‐based computing circuits. Thus far, most research has focused on FTJs with a perovskite oxide ferroelectric tunnel barrier. As the need for high‐temperature epitaxial film growth challenges the technological application of such inorganic junctions, more easily processable organic ferroelectrics can serve as alternative if large tunneling electroresistance (TER) and good switching durability would persist. This study reports on the performance of FTJs with a spin‐coated ferroelectric P(VDF‐TrFE) copolymer tunnel barrier. The use of three different bottom electrodes, indium tin oxide (ITO), La_0.67Sr_0.33MnO₃, (LSMO), and Nb‐doped SrTiO₃ (STO) are compared and it is shown that the polarity and magnitude of the TER effect depend on their conductivity. The largest TER of up to 10⁷% at room temperature is measured on FTJs with a semiconducting Nb‐doped STO electrode. This large switching effect is attributed to the formation of an extra barrier over the space charge region in the substrate. The organic FTJs exhibit good resistance retention and switching endurance up to 380 K, which is just below the ferroelectric Curie temperature of the P(VDF‐TrFE) barrier.     

A High‐k Fluorinated P(VDF‐TrFE)‐g‐PMMA Gate Dielectric for High‐Performance Flexible Field‐Effect Transistors

A newly synthesized high‐k polymeric insulator for use as gate dielectric layer for organic field‐effect transistors (OFETs) obtained by grafting poly(methyl methacrylate) (PMMA) in poly(vinylidene fluoride‐trifluoroethylene) (P(VDF‐TrFE)) via atom transfer radical polymerization transfer is reported. This material design concept intents to tune the electrical properties of the gate insulating layer (capacitance, leakage current, breakdown voltage, and operational stability) of the high‐k fluorinated polymer dielectric without a large increase in operating voltage by incorporating an amorphous PMMA as an insulator. By controlling the grafted PMMA percentage, an optimized P(VDF‐TrFE)‐g‐PMMA with 7 mol% grafted PMMA showing reasonably high capacitance (23–30 nF cm^?2) with low voltage operation and negligible current hysteresis is achieved. High‐performance low‐voltage‐operated top‐gate/bottom‐contact OFETs with widely used high mobility polymer semiconductors, poly[[2,5‐bis(2‐octyldodecyl)‐2,3,5,6‐tetrahydro‐3,6‐dioxopyrrolo [3,4‐c]pyrrole‐1,4‐diyl]‐alt‐[[2,2′‐(2,5‐thiophene)bis‐thieno(3,2‐b)thiophene]‐5,5′‐diyl]] (DPPT‐TT), and poly([N,N′‐bis(2‐octyldodecyl)‐naphthalene‐1,4,5,8‐bis(dicarboximide)‐2,6‐diyl]‐alt‐5,5′‐(2,2′‐bithiophene)) are demonstrated here. DPPT‐TT OFETs with P(VDF‐TrFE)‐g‐PMMA gate dielectrics exhibit a reasonably high field‐effect mobility of over 1 cm² V^?1 s^?1 with excellent operational stability.     

Nano‐Imprinted Ferroelectric Polymer Nanodot Arrays for High Density Data Storage

Ferroelectric vinylidene fluoride‐trifluoroethylene copolymer [P(VDF‐TrFE)] free‐standing ultrahigh density (≈75 Gb inch^?2) nanodot arrays are successfully fabricated through a facile, high‐throughput, and cost‐effective nano‐imprinting method using disposable anodic aluminum oxide with orderly arranged nanometer‐scale pores as molds. The nanodots show a large‐area smooth surface morphology, and the piezoresponse in each nanodot is strong and uniform. The preferred orientation of the copolymer chains in the nanodot arrays is favorable for polarization switching of single nanodots. The ferroelectric polymer memory prototype can be operated by a few volts with high writing/erasing speed, which comply with the requirements of integrated circuit. This approach provides a way of directly writing nanometer electronic features in two dimensions by piezoresponse force microscopy probe based technology, which is attractive for high density data storage.     

Sustainable Nanotextured Wave Energy Harvester Based on Ferroelectric Fatigue‐Free and Flexoelectricity‐Enhanced Piezoelectric P(VDF‐TrFE) Nanofibers with BaSrTiO3 Nanoparticles

Here, ultrathin, flexible, and sustainable nanofiber‐based piezoelectric nanogenerators (NF‐PENGs) are fabricated and applied as wave energy harvesters. The NF‐PENGs are composed of poly(vinylidene fluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)) nanofibers with embedded barium strontium titanate (BaSrTiO₃) nanoparticles, which are fabricated by using facile, scalable, and cost‐effective fiber‐forming methods, including electrospinning and solution blowing. The inclusion of ferroelectric BaSrTiO₃ nanoparticles inside the electrospun P(VDF‐TrFE) nanofibers enhances the sustainability of the NF‐PENGs and results in unique flexoelectricity‐enhanced piezoelectric nanofibers. Not only do these NF‐PENGs yield a superior performance compared to the previously reported NF‐PENGs, but they also exhibit an outstanding durability in terms of mechanical properties and cyclability. Furthermore, a new theoretical estimate of the energy harvesting efficiency from the water waves is introduced here, which can also be employed in future studies associated with various nanogenerators, including PENGs and triboelectric nanogenerators.     

Light‐Responsive Ion‐Redistribution‐Induced Resistive Switching in Hybrid Perovskite Schottky Junctions

Hybrid Perovskites have emerged as a class of highly versatile functional materials with applications in solar cells, photodetectors, transistors, and lasers. Recently, there have also been reports on perovskite‐based resistive switching (RS) memories, but there remain open questions regarding device stability and switching mechanism. Here, an RS memory based on a high‐quality capacitor structure made of an MAPbBr₃ (CH₃NH₃PbBr₃) perovskite layer sandwiched between Au and indium tin oxide (ITO) electrodes is reported. Such perovskite devices exhibit reliable RS with an ON/OFF ratio greater than 10³, endurance over 10³ cycles, and a retention time of 10⁴ s. The analysis suggests that the RS operation hinges on the migration of charged ions, most likely MA vacancies, which reversibly modifies the perovskite bulk transport and the Schottky barrier at the MAPbBr₃/ITO interface. Such perovskite memory devices can also be fabricated on flexible polyethylene terephthalate substrates with high bendability and reliability. Furthermore, it is found that reference devices made of another hybrid perovskite MAPbI₃ consistently exhibit filament‐type switching behavior. This work elucidates the important role of processing‐dependent defects in the charge transport of hybrid perovskites and provides insights on the ion‐redistribution‐based RS in perovskite memory devices.     

Large‐Area Silver‐Coated Silicon Nanowire Arrays for Molecular Sensing Using Surface‐Enhanced Raman Spectroscopy

A new and facile method to prepare large‐area silver‐coated silicon nanowire arrays for surface‐enhanced Raman spectroscopy (SERS)‐based sensing is introduced. High‐quality silicon nanowire arrays are prepared by a chemical etching method and used as a template for the generation of SERS‐active silver‐coated silicon nanowire arrays. The morphologies of the silicon nanowire arrays and the type of silver‐plating solution are two key factors determining the magnitude of SERS signal enhancement and the sensitivity of detection; they are investigated in detail for the purpose of optimization. The optimized silver‐coated silicon nanowire arrays exhibit great potential for ultrasensitive molecular sensing in terms of high SERS signal enhancement ability, good stability, and reproducibility. Their further applications in rapidly detecting molecules relating to human health and safety are discussed. A 10 s data acquisition time is capable of achieving a limit of detection of approximately 4 × 10^?6 M calcium dipicolinate (CaDPA), a biomarker for anthrax. This value is 1/15 the infectious dose of spores (6 × 10^?5 M required), revealing that the optimized silver‐coated silicon nanowire arrays as SERS‐based ultrasensitive sensors are extremely suitable for detecting Bacillus anthracis spores.     

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.     

Flexible and Transparent Nanocomposite of Reduced Graphene Oxide and P(VDF‐TrFE) Copolymer for High Thermal Responsivity in a Field‐Effect Transistor

A new class of temperature‐sensing materials is demonstrated along with their integration into transparent and flexible field‐effect transistor (FET) temperature sensors with high thermal responsivity, stability, and reproducibility. The novelty of this particular type of temperature sensor is the incorporation of an R‐GO/P(VDF‐TrFE) nanocomposite channel as a sensing layer that is highly responsive to temperature, and is optically transparent and mechanically flexible. Furthermore, the nanocomposite sensing layer is easily coated onto flexible substrates for the fabrication of transparent and flexible FETs using a simple spin‐coating method. The transparent and flexible nanocomposite FETs are capable of detecting an extremely small temperature change as small as 0.1 °C and are highly responsive to human body temperature. Temperature responsivity and optical transmittance of transparent nanocomposite FETs were adjustable and tuneable by changing the thickness and R‐GO concentration of the nanocomposite.     

Processing and Low Voltage Switching of Organic Ferroelectric Phase‐Separated Bistable Diodes

The processing of solution‐based binary blends of the ferroelectric random copolymer poly(vinylidene fluoride‐trifluoroethylene) P(VDF‐TrFE) and the semiconducting polymer poly(9,9‐dioctylfluorenyl‐2,7‐diyl) (PFO) applied by spin‐coating and wire‐bar coating is investigated. By systematic variation of blend composition, solvent, and deposition temperature it is shown that much smoother blend films can be obtained than reported thus far. At a low PFO:P(VDF‐TrFE) ratio the blend film consists of disk‐shaped PFO domains embedded in a P(VDF‐TrFE) matrix, while an inverted structure is obtained in case the P(VDF‐TrFE) is the minority component. The microstructure of the phase separated blend films is self‐affine. From this observation and from the domain size distribution it is concluded that the phase separation occurs via spinodal decomposition, irrespectively of blend ratio. This is explained by the strong incompatibility of the two polymers expressed by the binary phase diagram, as constructed from thermal analysis data. Time resolved numerical simulation of the microstructure evolution during de‐mixing qualitatively shows how an elevated deposition temperature has a smoothening effect as a result of the reduction of the repulsion between the blend components. The small roughness allowed the realization of bistable rectifying diodes that switch at low voltages with a yield of 100%. This indicates that memory characteristics can be tailored from the outset while processing parameters can be adjusted according to the phase behavior of the active components.     

A Skin‐Inspired Substrate with Spaghetti‐Like Multi‐Nanofiber Network of Stiff and Elastic Components for Stretchable Electronics

Mimicking the skin's non‐linear self‐limiting mechanical characteristics is of great interest. Skin is soft at low strain but becomes stiff at high strain and thereby can protect human tissues and organs from high mechanical loads. Herein, the design of a skin‐inspired substrate is reported based on a spaghetti‐like multi‐nanofiber network (SMNN) of elastic polyurethane (PU) nanofibers (NFs) sandwiched between stiff poly(vinyldenefluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)) NFs layers embedded in polydimethylsiloxane elastomer. The elastic moduli of the stretchable skin‐inspired substrate can be tuned in a range that matches well with the mechanical properties of skins by adjusting the loading ratios of the two NFs. Confocal imaging under stretching indicates that PU NFs help maintain the stretchability while adding stiff P(VDF‐TrFE) NFs to control the self‐limiting characteristics. Interestingly, the Au layer on the substrate indicates a negligible change in the resistance under cyclic (up to 7000 cycles at 35% strain) and dynamic stretching (up to 35% strain), which indicates the effective absorption of stress by the SMNN. A stretchable chemoresistive gas sensor on the skin‐inspired substrate also demonstrates a reasonable stability in NO₂ sensing response under strain up to 30%. The skin‐inspired substrate with SMNN provides a step toward ultrathin stretchable electronics.     

High‐Speed,Low‐Voltage,and Environmentally Stable Operation of Electrochemically Gated Zinc Oxide Nanowire Field‐Effect Transistors

Single‐crystal, 1D nanostructures are well known for their high mobility electronic transport properties. Oxide‐nanowire field‐effect transistors (FETs) offer both high optical transparency and large mechanical conformability which are essential for flexible and transparent display applications. Whereas the “on‐currents” achieved with nanowire channel transistors are already sufficient to drive active matrix organic light emitting diode (AMOLED) displays; it is shown here that incorporation of electrochemical‐gating (EG) to nanowire electronics reduces the operation voltage to ≤2 V. This opens up new possibilities of realizing flexible, portable, transparent displays that are powered by thin film batteries. A composite solid polymer electrolyte (CSPE) is used to obtain all‐solid‐state FETs with outstanding performance; the field‐effect mobility, on/off current ratio, transconductance, and subthreshold slope of a typical ZnO single‐nanowire transistor are 62 cm²/Vs, 10⁷, 155 μS/μm and 115 mV/dec, respectively. Practical use of such electrochemically‐gated field‐effect transistor (EG FET) devices is supported by their long‐term stability in air. Moreover, due to the good conductivity (≈10^?2 S/cm) of the CSPE, sufficiently high switching speed of such EG FETs is attainable; a cut‐off frequency in excess of 100 kHz is measured for in‐plane FETs with large gate‐channel distance of >10 μm. Consequently, operation speeds above MHz can be envisaged for top‐gate transistor geometries with insulator thicknesses of a few hundreds of nanometers. The solid polymer electrolyte developed in this study has great potential in future device fabrication using all‐solution processed and high throughput techniques.     

Stable α‐CsPbI3 Perovskite Nanowire Arrays with Preferential Crystallographic Orientation for Highly Sensitive Photodetectors

All‐inorganic metal‐halide perovskites CsPbX₃ (X = Cl, Br, I) exhibit higher stability than their organic–inorganic hybrid counterparts, but the thermodynamically instable perovskite α phase at room temperature of CsPbI₃ restricts the practical optoelectronic applications. Although the stabilization of α‐CsPbI₃ polycrystalline thin films is extensively studied, the creation of highly crystalline micro/nanostructures of α‐CsPbI₃ with large grain size and suppressed grain boundary remains challenging, which impedes the implementations of α‐CsPbI₃ for lateral devices, such as photoconductor‐type photodetectors. In this work, stable α‐CsPbI₃ perovskite nanowire arrays are demonstrated with large grain size, high crystallinity, regulated alignment, and position by controlling the dewetting dynamics of precursor solution on an asymmetric‐wettability topographical template. The correlation between the higher photoluminescence (PL) intensity and longer PL lifetime indicates the nanowires exhibit stable α phase and suppressed trap density. The preferential (100) orientation is characterized by discrete diffraction spots in grazing incidence wide‐angle scattering patterns, suggesting the long‐range crystallographic order of these nanowires. Based on these high‐quality nanowire arrays, highly sensitive photodetectors are realized with a responsivity of 1294 A W^?1 and long‐term stability with 90% performance retention after 30‐day ambient storage.