High‐Performance Nonvolatile Transistor Memories of Pentacence Using the Green Electrets of Sugar‐based Block Copolymers and Their Supramolecules

Reported here are the nonvolatile electrical characteristics of pentacene‐based organic field‐effect transistor (OFET) memory devices created from the green electrets of sugar‐based block copolymer maltoheptaose‐block‐polystyrene (MH‐b‐PS), and their supramolecules with 1‐aminopyrene (APy). The very hydrophilic and abundant‐hydroxyl MH block is employed as a charge‐trapping site, while the hydrophobic PS block serves as a matrix as well as a tunneling layer. The orientation of the MH nanodomains could be well controlled in the PS matrix with random spheres, vertical cylinders, and ordered horizontal cylinders via increasing solvent annealing time, leading to different electrical switching characteristics. The electron‐trapping ability induced by the horizontal‐cylinder MH is stronger than those of the random‐sphere and vertical‐cylinder structures, attributed to the effective contact area. The electrical memory window of the device is further improved via the supramolecules of hydrogen‐bonding 1‐aminopyrene to the MH moieties of MH‐b‐PS for enhancing the hole‐trapping ability. The optimized device using the horizontal cylinders of the supramolecule electret exhibits the excellent memory characteristics of a wide memory window (52.7 V), retention time longer than 10⁴ s with a high ON/OFF ratio of >10⁵, and stable reversibility over 200 cycles. This study reveals a new approach to achieve a high‐performance flash memory through the morphology control of sugar‐based block copolymers and their supramolecules.     

Donor–Acceptor Poly(3‐hexylthiophene)‐block‐Pendent Poly(isoindigo) with Dual Roles of Charge Transporting and Storage Layer for High‐Performance Transistor‐Type Memory Applications

Field‐effect transistor memories usually require one additional charge storage layer between the gate contact and organic semiconductor channel. To avoid such complication, new donor–acceptor rod–coil diblock copolymers (P3HT₄₄‐b‐Piso_n) of poly(3‐hexylthiophene) (P3HT)‐block‐poly(pendent isoindigo) (Piso) are designed, which exhibit high performance transistor memory characteristics without additional charge storage layer. The P3HT and Piso blocks are acted as the charge transporting and storage elements, respectively. The prepared P3HT₄₄‐b‐Piso_n can be self‐assembled into fibrillar‐like nanostructures after the thermal annealing process, confirmed by atomic force microscopy and grazing‐incidence X‐ray diffraction. The lowest‐unoccupied molecular orbital levels of the studied polymers are significantly lowered as the block length of Piso increases, leading to a stronger electron affinity as well as charge storage capability. The field‐effect transistors (FETs) fabricated from P3HT₄₄‐b‐Piso_n possess p‐type mobilities up to 4.56 × 10^?2 cm² V^?1 s^?1, similar to that of the regioregular P3HT. More interestingly, the FET memory devices fabricated from P3HT₄₄‐b‐Piso_n exhibit a memory window ranging from 26 to 79 V by manipulating the block length of Piso, and showed stable long‐term data endurance. The results suggest that the FET characteristics and data storage capability can be effectively tuned simultaneously through donor/acceptor ratio and thin film morphology in the block copolymer system.     

Stretchable Active Matrix Inorganic Light‐Emitting Diode Display Enabled by Overlay‐Aligned Roll‐Transfer Printing

An active matrix‐type stretchable display is realized by overlay‐aligned transfer of inorganic light‐emitting diode (LED) and single‐crystal Si thin film transistor (TFT) with roll processes. The roll‐based transfer enables integration of heterogeneous thin film devices on a rubber substrate while preserving excellent electrical and optical properties of these devices, comparable to their bulk properties. The electron mobility of the integrated Si‐TFT is over 700 cm² V^?1 s^?1, and this is attributed to the good interface between the Si channel and the thermally grown SiO₂ insulator. The light emission properties of the LED are of wafer quality. The resulting display stably operates under tensile strains up to 40%, over 200 cycles, demonstrating the potential of stretchable displays based on inorganic materials.     

Self‐Assembled Nanowires of Organic n‐Type Semiconductor for Nonvolatile Transistor Memory Devices

Organic nonvolatile transistor‐type memory (ONVM) devices are developed using self‐assembled nanowires of n‐type semiconductor, N,N′‐bis(2‐phenylethyl)‐perylene‐3,4:9,10‐tetracarboxylic diimide (BPE‐PTCDI). The effects of nanowire dimension and silane surface treatment on the memory characteristics are explored. The diameter of the nanowires is reduced by increasing the non‐solvent methanol composition, which led to the enhanced crystallinity and high field‐effect mobility. The BPE‐PTCDI nanowires with small diameters induce high electrical fields and result in a large memory window (the shifting of the threshold voltage, ΔV_th). The ΔV_th value of BPE‐PTCDI nanowire based ONVM device on the bare substrate can reach 51 V, which is significantly larger than that of thin film. The memory window is further enhanced to 78 V with the on/off ratio of 2.1 × 10⁴ and the long retention time (10⁴ s), using a hydrophobic surface (such as trichloro(phenyl)silane‐treated surface). The above results demonstrate that the n‐type semiconducting nanowires have potential applications in high performance non‐volatile transistor memory devices.     

Resistive Switching Memory Integrated with Nanogenerator for Self‐Powered Bioimplantable Devices

Resistive random access memory (ReRAM) devices powered by piezoelectric nanogenerators (NGs) have been investigated for their application to future implantable biomedical devices. Biocompatible (Na_0.5K_0.5)NbO₃ (NKN) films that are grown at 300 °C on TiN/SiO₂/Si and flexible TiN/Polyimide (TiN‐PI) substrates are used for ReRAM and NGs, respectively. These NKN films have an amorphous phase containing NKN nanocrystals with a size of 5.0 nm. NKN ReRAM devices exhibit typical bipolar switching behavior that can be explained by the formation and rupture of oxygen‐vacancy filaments. They have good ReRAM properties such as a large ratio of R_HRS to R_LRS as well as high reliability. The NKN film grown on flexible TiN‐PI substrate exhibits a high piezoelectric strain constant of 50 pm V^?1. The NKN NG has a large open‐circuit output voltage of 2.0 V and a short‐circuit output current of 40 nA, which are sufficient to drive NKN ReRAM devices. Stable switching properties with a large ON/OFF ratio of 10² are obtained from NKN ReRAM driven by NKN NG.     

Highly Stretchable,High‐Mobility,Free‐Standing All‐Organic Transistors Modulated by Solid‐State Elastomer Electrolytes

Highly stretchable, high‐mobility, and free‐standing coplanar‐type all‐organic transistors based on deformable solid‐state elastomer electrolytes are demonstrated using ionic thermoplastic polyurethane (i‐TPU), thereby showing high reliability under mechanical stimuli as well as low‐voltage operation. Unlike conventional ionic dielectrics, the i‐TPU electrolyte prepared herein has remarkable characteristics, i.e., a large specific capacitance of 5.5 µF cm^?2, despite the low weight ratio (20 wt%) of the ionic liquid, high transparency, and even stretchability. These i‐TPU‐based organic transistors exhibit a mobility as high as 7.9 cm² V^?1 s^?1, high bendability (R_c, radius of curvature: 7.2 mm), and good stretchability (60% tensile strain). Moreover, they are suitable for low‐voltage operation (V_DS = ?1.0 V, V_GS = ?2.5 V). In addition, the electrical characteristics such as mobility, on‐current, and threshold voltage are maintained even in the concave and convex bending state (bending tensile strain of ≈3.4%), respectively. Finally, free‐standing, fully stretchable, and semi‐transparent coplanar‐type all‐organic transistors can be fabricated by introducing a poly(3,4‐ethylenedioxythiophene):polystyrene sulfonic acid layer as source/drain and gate electrodes, thus achieving low‐voltage operation (V_DS = ?1.5 V, V_GS = ?2.5 V) and an even higher mobility of up to 17.8 cm² V^?1 s^?1. Moreover, these devices withstand stretching up to 80% tensile strain.     

Self Encapsulated Poly(3‐hexylthiophene)‐poly(fluorinated alkyl methacrylate) Rod‐Coil Block Copolymers with High Field Effect Mobilities on Bare SiO2

Conjugated rod‐coil block copolymers provide an interesting route towards enhancing the properties of the conjugated block due to self‐assembly and the interplay of rod‐rod and rod‐coil interactions. Here, we demonstrate the ability of an attached semi‐fluorinated block to significantly improve upon the charge carrier properties of regioregular poly(3‐hexyl thiophene) (rr‐P3HT) materials on bare SiO₂. The thin film hole mobilities on bare SiO₂ dielectric surfaces of poly (3‐hexyl thiophene)‐block‐polyfluoromethacrylates (P3HT‐b‐PFMAs) can approach up to 0.12 cm² V^?1 s^?1 with only 33 wt% of the P3HT block incorporated in the copolymer, as compared to rr‐P3HT alone which typically has mobilities averaging 0.03 cm² V^?1 s^?1. To our knowledge, this is the highest mobility reported in literature for block copolymers containing a P3HT. More importantly, these high hole mobilities are achieved without multistep OTS treatments, argon protection, or post‐annealing conditions. Grazing incidence wide‐angle x‐ray scattering (GIWAX) data revealed that in the P3HT‐b‐PFMA copolymers, the P3HT rod block self‐assembles into highly ordered lamellar structures, similar to that of the rr‐P3HT homopolymer. Grazing incidence small‐angle x‐ray scattering (GISAXS) data revealed that lamellar structures are only observed in perpendicular direction with short PFMA blocks, while lamellae in both perpendicular and parallel directions are observed in polymers with longer PFMA blocks. AFM, GIWAXS, and contact angle measurements also indicate that PFMA block assembles at the polymer thin film surface and forms an encapsulation layer. The high charge carrier mobilities and the hydrophobic surface of the block copolymer films clearly demonstrates the influence of the coil block segment on device performance by balancing the crystallization and microphase separation in the bulk morphological structure.     

Substrate‐Dependent Spin–Orbit Coupling in Hybrid Perovskite Thin Films

Solution‐processing hybrid metal halide perovskites are promising materials for developing flexible thin‐film devices. This work reports the substrate effects on the spin–orbit coupling (SOC) in perovskite films through thermal expansion under thermal annealing. X‐ray diffraction (XRD) measurements show that using a flexible polyethylene naphthalate (PEN) substrate introduces a smaller mechanical strain in perovskite MAPbI_3?xCl_x films, as compared to conventional glass substrates. Interestingly, the linear/circular photoexcitation‐modulated photocurrent studies find that decreasing mechanical strain gives rise to a weaker orbit–orbit interaction toward decreasing the SOC in the MAPbI_3?xCl_x films prepared on flexible PEN substrates relative to rigid glass substrates. Simultaneously, decreasing the mechanical strain causes a reduction in the internal magnetic parameter inside the MAPbI_3?xCl_x films, providing further evidence to show that introducing mechanical strain can affect the SOC in hybrid perovskite films upon using flexible substrates toward developing flexible perovskite thin‐film devices. Furthermore, thermal admittance spectroscopy indicates that the trap states are increased in the perovskite films prepared on flexible PEN substrates as compared to glass substrates. Consequently, PEN and rigid glass substrates lead to shorter and longer photoluminescence lifetimes, respectively. Clearly, these findings provide an insightful understanding on substrate effects on optoelectronic properties in flexible perovskite thin‐film devices.     

Wide Bandgap Copolymers Based on Quinoxalino[6,5‐f].quinoxaline for Highly Efficient Nonfullerene Polymer Solar Cells

Two novel wide bandgap copolymers based on quinoxalino[6,5‐f]quinoxaline (NQx) acceptor block, PBDT–NQx and PBDTS–NQx, are successfully synthesized for efficient nonfullerene polymer solar cells (PSCs). The attached conjugated side chains on both benzodithiophene (BDT) and NQx endow the resulting copolymers with low‐lying highest occupied molecular orbital (HOMO) levels. The sulfur atom insertion further reduces the HOMO level of PBDTS–NQx to ?5.31 eV, contributing to a high open‐circuit voltage, V _oc, of 0.91 V. Conjugated n ‐octylthienyl side chains attached on the NQx skeletons also significantly improve the π–π* transitions and optical absorptions of the copolymers in the region of short wavelengths, which induce a good complementary absorption when blending with the low bandgap small molecular acceptor of 3,9‐bis(2‐methylene‐(3‐(1,1‐dicyanomethylene)‐indanone))‐5,5,11,11‐tetrakis(4‐hexylphenyl)‐dithieno[2,3‐d:2′,3′‐d′]‐s‐indaceno[1,2‐b:5,6‐b′]dithiophene. The wide absorption range makes the active blends absorb more photons, giving rise to a high short‐circuit current density, J _sc, value of 15.62 mA cm^?2. The sulfur atom insertion also enhances the crystallinity of PBDTS–NQx and presents its blend film with a favorable nanophase separation, resulting in improved J _sc and fill factor (FF) values with a high power conversion efficiency of 11.47%. This work not only provides a new fused ring acceptor block (NQx) for constructing high‐performance wide bandgap copolymers but also provides the NQx‐based copolymers for achieving highly efficient nonfullerene PSCs.     

Synthesis,Morphology, and Properties of Poly(3‐hexylthiophene)‐block‐Poly(vinylphenyl oxadiazole) Donor–Acceptor Rod–Coil Block Copolymers and Their Memory Device Applications

Novel donor–acceptor rod–coil diblock copolymers of regioregular poly(3‐hexylthiophene) ( P3HT )‐block‐poly(2‐phenyl‐5‐(4‐vinylphenyl)‐1,3,4‐oxadiaz‐ole) ( POXD ) are successfully synthesized by the combination of a modified Grignard metathesis reaction ( GRIM ) and atom transfer radical polymerization ( ATRP ). The effects of the block ratios of the P3HT donor and POXD pendant acceptor blocks on the morphology, field effect transistor mobility, and memory device characteristics are explored. The TEM, SAXS, WAXS, and AFM results suggest that the coil block fraction significantly affects the chain packing of the P3HT block and depresses its crystallinity. The optical absorption spectra indicate that the intramolecular charge transfer between the main chain P3HT donor and the side chain POXD acceptor is relatively weak and the level of order of P3HT chains is reduced by the incorporation of the POXD acceptor. The field effect transistor (FET) hole mobility of the system exhibits a similar trend on the optical properties, which are also decreased with the reduced ordered P3HT crystallinity. The low‐lying highest occupied molecular orbital (HOMO) energy level (–6.08 eV) of POXD is employed as charge trap for the electrical switching memory devices. P3HT‐ b ‐POXD exhibits a non‐volatile bistable memory or insulator behavior depending on the P3HT / POXD block ratio and the resulting morphology. The ITO/ P3HT₄₄ ‐b‐ POXD₁₈ /Al memory device shows a non‐volatile switching characteristic with negative differential resistance (NDR) effect due to the charge trapped POXD block. These experimental results provide the new strategies for the design of donor‐acceptor rod‐coil block copolymers for controlling morphology and physical properties as well as advanced memory device applications.     

Network Structure Modification‐Enabled Hybrid Polymer Dielectric Film with Zirconia for the Stretchable Transistor Applications

Stretchable electronic devices should be enabled by the smart design of materials and architectures because their commercialization is limited by the tradeoff between stretchability and electrical performance limits. In this study, thin‐film transistors are fabricated using strategies that combine the unit process of a novel hybrid gate insulator and low‐temperature indium gallium tin oxide (IGTO) channel layer and a stress‐relief substrate structure. Novel hybrid dielectric films are synthesized and their molecular structural configurations are analyzed. These films consist of a polymer [poly(4‐vinylphenol‐co‐methylmethacrylate)], cross‐linkers having different binding structures [1,6‐bis(trimethoxysilyl)hexane (BTMSH), dodecyltrimethoxysilane, and poly(melamine‐co‐formaldehyde)], and an inorganic zirconia component (ZrO_x). The hybrid film with BTMSH cross‐linker and 0.2 M ZrO_x exhibits excellent insulating properties as well as mechanical stretchability. IGTO transistors fabricated on polyimide‐coated glass substrates are transferred to the rubber substrate to offer stretchability of the transistor pixelated thin‐film transistors. IGTO transistors fabricated on stretchable substrates using these strategies show promising electrical performance and mechanical durability. After 200 stretchability test cycles under uniaxial elongation of approximately 300%, the IGTO transistor still retains a high carrier mobility of 21.7 cm² V^?1 s^?1, a low sub‐threshold gate swing of 0.68 V decade^?1 and a high I_ON/OFF ratio of 2.0 × 10⁷.     

Vertical Orientation of Nanodomains on Versatile Substrates through Self‐Neutralization Induced by Star‐Shaped Block Copolymers

Vertical orientation of lamellar and cylindrical nanodomains of block copolymers on substrates is one of the most promising means for developing nanopatterns of next‐generation microelectronics and storage media. However, parallel orientation of lamellar and cylindrical nanodomains is generally preferred due to different affinity between two block segments in a block copolymer toward the substrate and/or air. Thus, vertical orientation of the nanodomains is only obtained under various pre‐ or post‐treatments such as surface neutralization by random copolymers, solvent annealing, and electric or magnetic field. Here, a novel self‐neutralization concept is introduced by designing molecular architecture of a block copolymer. Star‐shaped 18 arm poly(methyl methacrylate)‐block‐polystyrene copolymers ((PMMA‐b‐PS)₁₈) exhibiting lamellar and PMMA cylindrical nanodomains are synthesized. When a thin film of (PMMA‐b‐PS)₁₈ is spin‐coated on a substrate, vertically aligned lamellar and cylindrical nanodomains are obtained without any pre‐ or post‐treatment, although thermal annealing for a short time (less than 30 min) is required to improve the spatial array of vertically aligned nanodomains. This result is attributed to the star‐shaped molecular architecture that overcomes the difference in the surface affinity between PS and PMMA chains. Moreover, vertical orientations are observed on versatile substrates, for instance, semiconductor (Si, SiO_x), metal (Au), PS or PMMA‐brushed substrate, and a flexible polymer sheet of polyethylene naphthalate.     

Ferroelastic Strain Induced Antiferroelectric‐Ferroelectric Phase Transformation in Multilayer Thin Film Structures

Coupling effects among mechanical, electrical and magnetic parameters in thin film structures including ferroic thin films provide exciting opportunity for creating device functionalities. For thin films deposited on a substrate, their mechanical stress and microstructure are usually determined by the composition and processing of the films and the lattice and thermal mismatch with the substrate. Here it is found that the stress and structure of an antiferroelectric (Pb_0.97,La_0.02)(Zr_0.90,Sn_0.05,Ti_0.05)O₃ (PLZST) thin film are changed completely by a ferroelastic strain in a magnetic shape memory (MSM) alloy Ni‐Mn‐Ga (NMG) thin film on the top of the PLZST, despite the existence of the substrate constraint. The ferroelastic strain in the NMG film results in antiferroelectric (AFE) to ferroelectric (FE) phase transformation in the PLZST layer underneath. This finding indicates a different strategy to modulate the structure and function for multilayer thin films and to create unprecedented devices with ferroic thin films.     

Printed,Flexible, Organic Nano‐Floating‐Gate Memory: Effects of Metal Nanoparticles and Blocking Dielectrics on Memory Characteristics

The effects of using a blocking dielectric layer and metal nanoparticles (NPs) as charge‐trapping sites on the characteristics of organic nano‐floating‐gate memory (NFGM) devices are investigated. High‐performance NFGM devices are fabricated using the n‐type polymer semiconductor, poly{[N,N′‐bis(2‐octyldodecyl)‐naphthalene‐1,4,5,8‐bis(dicarboximide)‐2,6‐diyl]‐alt‐5,5′‐(2,2′‐bithiophene)} (P(NDI2OD‐T2)), and various metal NPs. These NPs are embedded within bilayers of various polymer dielectrics (polystyrene (PS)/poly(4‐vinyl phenol) (PVP) and PS/poly(methyl methacrylate) (PMMA)). The P(NDI2OD‐T2) organic field‐effect transistor (OFET)‐based NFGM devices exhibit high electron mobilities (0.4–0.5 cm² V^?1 s^?1) and reliable non‐volatile memory characteristics, which include a wide memory window (≈52 V), a high on/off‐current ratio (I_on/I_off ≈ 10⁵), and a long extrapolated retention time (>10⁷ s), depending on the choice of the blocking dielectric (PVP or PMMA) and the metal (Au, Ag, Cu, or Al) NPs. The best memory characteristics are achieved in the ones fabricated using PMMA and Au or Ag NPs. The NFGM devices with PMMA and spatially well‐distributed Cu NPs show quasi‐permanent retention characteristics. An inkjet‐printed flexible P(NDI2OD‐T2) 256‐bit transistor memory array (16 × 16 transistors) with Au‐NPs on a polyethylene naphthalate substrate is also fabricated. These memory devices in array exhibit a high I_on/I_off (≈10^{4 ± 0.85}), wide memory window (≈43.5 V ± 8.3 V), and a high degree of reliability.     

Reversible Crumpling of 2D Titanium Carbide (MXene) Nanocoatings for Stretchable Electromagnetic Shielding and Wearable Wireless Communication

In the emerging Internet of Things, stretchable antennas can facilitate wireless communication between wearable and mobile electronic devices around the body. The proliferation of wireless devices transmitting near the human body also raises interference and safety concerns that demand stretchable materials capable of shielding electromagnetic interference (EMI). Here, an ultrastretchable conductor is fabricated by depositing a crumple‐textured coating composed of 2D Ti₃C₂T_x nanosheets (MXene) and single‐walled carbon nanotubes (SWNTs) onto latex, which can be fashioned into high‐performance wearable antennas and EMI shields. The resulting MXene‐SWNT (S‐MXene)/latex devices are able to sustain up to an 800% areal strain and exhibit strain‐insensitive resistance profiles during a 500‐cycle fatigue test. A single layer of stretchable S‐MXene conductors demonstrate a strain‐invariant EMI shielding performance of ≈30 dB up to 800% areal strain, and the shielding performance is further improved to ≈47 and ≈52 dB by stacking 5 and 10 layers of S‐MXene conductors, respectively. Additionally, a stretchable S‐MXene dipole antenna is fabricated, which can be uniaxially stretched to 150% with unaffected reflected power <0.1%. By integrating S‐MXene EMI shields with stretchable S‐MXene antennas, a wearable wireless system is finally demonstrated that provides mechanically stable wireless transmission while attenuating EM absorption by the human body.     

Dithienocarbazole‐Based Ladder‐Type Heptacyclic Arenes with Silicon,Carbon, and Nitrogen Bridges: Synthesis,Molecular Properties,Field‐Effect Transistors,and Photovoltaic Applications

A new class of ladder‐type dithienosilolo‐carbazole ( DTSC ), dithienopyrrolo‐carbazole ( DTPC ), and dithienocyclopenta‐carbazole ( DTCC ) units is developed in which two outer thiophene subunits are covalently fastened to the central 2,7‐carbazole cores by silicon, nitrogen, and carbon bridges, respectively. The heptacyclic multifused monomers are polymerized with the benzothiadiazole ( BT ) acceptor by palladium‐catalyzed cross‐coupling to afford three alternating donor‐acceptor copolymers poly(dithienosilolo‐carbazole‐alt‐benzothiadiazole) ( PDTSCBT) , poly(dithienocyclopenta‐carbazole‐alt‐benzothiadiazole) ( PDTCCBT), and poly(dithienopyrrolo‐carbazole‐alt‐benzothiadiazole) ( PDTPCBT) . The silole units in DTSC possess electron‐accepting ability that lowers the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) energy levels of PDTSCBT , whereas stronger electron‐donating ability of the pyrrole moiety in DTPC increases the HOMO and LUMO energy levels of PDTPCBT . The optical bandgaps (E_g^opt) deduced from the absorption edges of thin film spectra are in the following order: PDTSCBT (1.83 eV) > PDTCCBT (1.64 eV) > PDTPCBT (1.50 eV). This result indicated that the donor strength of the heptacyclic arenes is in the order: DTPC > DTCC > DTSC . The devices based on PDTSCBT and PDTCCBT exhibited high hole mobilities of 0.073 and 0.110 cm² V^?1 s^?1, respectively, which are among the highest performance from the OFET devices based on the amorphous donor‐acceptor copolymers. The bulk heterojunction photovoltaic device using PDTSCBT as the p‐type material delivered a promising efficiency of 5.2% with an enhanced open circuit voltage, V_oc, of 0.82 V.     

Efficient Conjugated‐Polymer Optoelectronic Devices Fabricated by Thin‐Film Transfer‐Printing Technique

The fabrication of functional multilayered conjugated‐polymer structures with well‐defined organic‐organic interfaces for optoelectronic‐device applications is constrained by the common solubility of many polymers in most organic solvents. Here, we report a simple, low‐cost, large‐area transfer‐printing technique for the deposition and patterning of conjugated‐polymer thin films. This method utilises a planar poly(dimethylsiloxane) (PDMS) stamp, along with a water‐soluble sacrificial layer, to pick up an organic thin film (～20 nm to 1 µm) from a substrate and subsequently deliver this film to a target substrate. We demonstrate the versatility of this transfer‐printing technique and its applicability to optoelectronic devices by fabricating bilayer structures of poly(9,9‐di‐n‐octylfluorene‐alt‐(1,4‐phenylene‐((4‐sec‐butylphenyl)imino)‐1,4‐phenylene))/poly(9,9‐di‐n‐octylfluorene‐alt‐benzothiadiazole) (TFB/F8BT) and poly(3‐hexylthiophene)/methanofullerene([6,6]‐phenyl C₆₁ butyric acid methyl ester) (P3HT/PCBM), and incorporating them into light‐emitting diodes (LEDs) and photovoltaic (PV) cells, respectively. For both types of device, bilayer devices fabricated with this transfer‐printing technique show equal, if not superior, performance to either blend devices or bilayer devices fabricated by other techniques. This indicates well‐controlled organic‐organic interfaces achieved by the transfer‐printing technique. Furthermore, this transfer‐printing technique allows us to study the nature of the excited states and the transport of charge carriers across well‐defined organic interfaces, which are of great importance to organic electronics.     

Interface‐Engineered Amorphous TiO2‐Based Resistive Memory Devices

Crossbar‐type bipolar resistive memory devices based on low‐temperature amorphous TiO₂ (a‐TiO₂) thin films are very promising devices for flexible nonvolatile memory applications. However, stable bipolar resistive switching from amorphous TiO₂ thin films has only been achieved for Al metal electrodes that can have severe problems like electromigration and breakdown in real applications and can be a limiting factor for novel applications like transparent electronics. Here, amorphous TiO₂‐based resistive random access memory devices are presented that universally work for any configuration of metal electrodes via engineering the top and bottom interface domains. Both by inserting an ultrathin metal layer in the top interface region and by incorporating a thin blocking layer in the bottom interface, more enhanced resistance switching and superior endurance performance can be realized. Using high‐resolution transmission electron microscopy, point energy dispersive spectroscopy, and energy‐filtering transmission electron microscopy, it is demonstrated that the stable bipolar resistive switching in metal/a‐TiO₂/metal RRAM devices is attributed to both interface domains: the top interface domain with mobile oxygen ions and the bottom interface domain for its protection against an electrical breakdown.     

All‐Solution‐Processed Indium‐Free Transparent Composite Electrodes based on Ag Nanowire and Metal Oxide for Thin‐Film Solar Cells

Fully solution‐processed Al‐doped ZnO/silver nanowire (AgNW)/Al‐doped ZnO/ZnO multi‐stacked composite electrodes are introduced as a transparent, conductive window layer for thin‐film solar cells. Unlike conventional sol–gel synthetic pathways, a newly developed combustion reaction‐based sol–gel chemical approach allows dense and uniform composite electrodes at temperatures as low as 200 °C. The resulting composite layer exhibits high transmittance (93.4% at 550 nm) and low sheet resistance (11.3 Ω sq^‐1), which are far superior to those of other solution‐processed transparent electrodes and are comparable to their sputtered counterparts. Conductive atomic force microscopy reveals that the multi‐stacked metal‐oxide layers embedded with the AgNWs enhance the photocarrier collection efficiency by broadening the lateral conduction range. This as‐developed composite electrode is successfully applied in Cu(In_1‐x,Ga_x)S₂ (CIGS) thin‐film solar cells and exhibits a power conversion efficiency of 11.03%. The fully solution‐processed indium‐free composite films demonstrate not only good performance as transparent electrodes but also the potential for applications in various optoelectronic and photovoltaic devices as a cost‐effective and sustainable alternative electrode.     

Air‐Stable Cesium Lead Iodide Perovskite for Ultra‐Low Operating Voltage Resistive Switching

CsPbX₃ (X = halide, Cl, Br, or I) all‐inorganic halide perovskites (IHPs) are regarded as promising functional materials because of their tunable optoelectronic characteristics and superior stability to organic–inorganic hybrid halide perovskites. Herein, nonvolatile resistive switching (RS) memory devices based on all‐inorganic CsPbI₃ perovskite are reported. An air‐stable CsPbI₃ perovskite film with a thickness of only 200 nm is successfully synthesized on a platinum‐coated silicon substrate using low temperature all‐solution process. The RS memory devices of Ag/polymethylmethacrylate (PMMA)/CsPbI₃/Pt/Ti/SiO₂/Si structure exhibit reproducible and reliable bipolar switching characteristics with an ultralow operating voltage (<+0.2 V), high on/off ratio (>10⁶), reversible RS by pulse voltage operation (pulse duration < 1 ms), and multilevel data storage. The mechanical flexibility of the CsPbI₃ perovskite RS memory device on a flexible substrate is also successfully confirmed. With analyzing the influence of phase transition in CsPbI₃ on RS characteristics, a mechanism involving conducting filaments formed by metal cation migration is proposed to explain the RS behavior of the memory device. This study will contribute to the understanding of the intrinsic characteristics of IHPs for low‐voltage resistive switching and demonstrate the huge potential of them for use in low‐power consumption nonvolatile memory devices on next‐generation computing systems.