Selenium-alloyed tellurium oxide for amorphous p-channel transistors.

Compared to polycrystalline semiconductors, amorphous semiconductors offer inherent cost-effective, simple and uniform manufacturing. Traditional amorphous hydrogenated Si falls short in electrical properties, necessitating the exploration of new materials. The creation of high-mobility amorphous n-type metal oxides, such as a-InGaZnO (ref. 1), and their integration into thin-film transistors (TFTs) have propelled advancements in modern large-area electronics and new-generation displays2-8. However, finding comparable p-type counterparts poses notable challenges, impeding the progress of complementary metal-oxide-semiconductor technology and integrated circuits9-11. Here we introduce a pioneering design strategy for amorphous p-type semiconductors, incorporating high-mobility tellurium within an amorphous tellurium suboxide matrix, and demonstrate its use in high-performance, stable p-channel TFTs and complementary circuits. Theoretical analysis unveils a delocalized valence band from tellurium 5p bands with shallow acceptor states, enabling excess hole doping and transport. Selenium alloying suppresses hole concentrations and facilitates the p-orbital connectivity, realizing high-performance p-channel TFTs with an average field-effect hole mobility of around 15 cm2 V-1 s-1 and on/off current ratios of 106-107, along with wafer-scale uniformity and long-term stabilities under bias stress and ambient ageing. This study represents a crucial stride towards establishing commercially viable amorphous p-channel TFT technology and complementary electronics in a low-cost and industry-compatible manner.

Unlocking the Potential of Tin-Based Perovskites: Properties, Progress, and Applications in New-Era Electronics.

Electronics have greatly promoted the development of modern society and the exploration of new semiconducting materials with low cost and high mobility continues to attract interest in the advance of next-generation electronic devices. Among emerging semiconductors, the metal-halide perovskite, especially the nontoxic tin (Sn)-based candidates, has recently made breakthroughs in the field of diverse electronic devices due to its excellent charge transport properties and cost-effective large-area deposition capability at low temperatures. To enable a more comprehensive understanding of this emerging research field and promote the development of new-generation perovskite electronics, this review aims to provide an in-depth understanding with the discussion of unique physical properties of Sn-based perovskites and the summarization of recent research progress of Sn-based perovskite field-effect transistors (FETs) and diverse electronic devices. The unique character of negligible ion migration is also discussed, which is fundamentally different from the lead-based counterparts and provides a great prerequisite for device application. The following section highlights the potential broad applications of Sn-perovskite FETs as a competitive and feasible technology. Finally, an outlook and remaining challenges are given to advance the progression of Sn-based perovskite FETs, especially on the origin and solution of stability problems toward high-performance Sn-based perovskite electronics.

Synthesis and Characterization of Diketopyrrolopyrrole-Based Conjugated Polymers with Bithiophene and Biselenophene for Organic Thin Film Transistors.

In this study, two new thieno[3,2-b]thiophene-diketopyrrolopyrrole (DPP)-based polymers, poly{2,5-bis(2-dodecylhexadecyl)-3,6-bis(thieno[3,2-b]thiophen-2-yl)pyrrolo[3,4-c]pyrrole-1,4(2H,5H)-dione-alt-2, 2'-bithiophene} (PTTDPP-BT) and {2,5-bis(2-dodecylhexadecyl)-3,6-bis(thieno[3,2-b]thiophen-2-yl) pyrrolo[3,4-c]pyrrole-1,4(2H,5H)-dione-alt-2,2'-selenophene} (PTTDPP-BSe), which contained bithiophene (BT) and biselenophene (BSe) units, respectively, were designed and synthesized. The introduction of BT and BSe units affected the optical, electrochemical, morphological, and charge transport properties of the polymers. Experimental results revealed that the frontier molecular orbital energy levels of PTTDPP-BT were slightly higher because of the relatively strong electron donating ability of the sulfur atom and the polymer also exhibited good solubility. The maximum mobility in the case of PTTDPP-BT at 250 °C was 0.068 cm² V-1 s-1 and that of PTTDPP-BSe was 0.029 cm² V-1 s-1 (at 200 °C).

Interfacial Engineering of Nanoporous Architectures in Ga2O3 Film toward Self-Aligned Tubular Nanostructure with an Enhanced Photocatalytic Activity on Water Splitting.

The present work demonstrates the formation of self-aligned nanoporous architecture of gallium oxide by anodization of gallium metal film controlled at -15 °C in aqueous electrolyte consisting of phosphoric acid. SEM examination of the anodized film reveals that by adding ethylene glycol to the electrolyte and optimizing the ratio of phosphoric acid and water, chemical etching at the oxide/electrolyte interfaces can be controlled, leading to the formation of aligned nanotubular oxide structures with closed bottom. XPS analysis confirms the chemical composition of the oxide film as Ga2O3. Further, XRD and SAED examination reveals that the as-synthesized nanotubular structure is amorphous, and can be crystallized to ß-Ga2O3 phase by annealing the film at 600 °C. The nanotubular structured film, when used as photoanode for photoelectrochemical splitting of water, achieved a higher photocurrent of about two folds than that of the nanoporous film, demonstrating the rewarding effect of the nanotubular structure. In addition, the work also demonstrates the formation of highly organized nonporous Ga2O3 structure on a nonconducting glass substrate coated with thin film of Ga-metal, highlighting that the current approach can be extended for the formation of self-organized nanoporous Ga2O3 thin film even on nonconducting flexible substrates.

Flexible metal-oxide devices made by room-temperature photochemical activation of sol-gel films.

Amorphous metal-oxide semiconductors have emerged as potential replacements for organic and silicon materials in thin-film electronics. The high carrier mobility in the amorphous state, and excellent large-area uniformity, have extended their applications to active-matrix electronics, including displays, sensor arrays and X-ray detectors. Moreover, their solution processability and optical transparency have opened new horizons for low-cost printable and transparent electronics on plastic substrates. But metal-oxide formation by the sol-gel route requires an annealing step at relatively high temperature, which has prevented the incorporation of these materials with the polymer substrates used in high-performance flexible electronics. Here we report a general method for forming high-performance and operationally stable metal-oxide semiconductors at room temperature, by deep-ultraviolet photochemical activation of sol-gel films. Deep-ultraviolet irradiation induces efficient condensation and densification of oxide semiconducting films by photochemical activation at low temperature. This photochemical activation is applicable to numerous metal-oxide semiconductors, and the performance (in terms of transistor mobility and operational stability) of thin-film transistors fabricated by this route compares favourably with that of thin-film transistors based on thermally annealed materials. The field-effect mobilities of the photo-activated metal-oxide semiconductors are as high as 14 and 7 cm(2) V(-1) s(-1) (with an Al(2)O(3) gate insulator) on glass and polymer substrates, respectively; and seven-stage ring oscillators fabricated on polymer substrates operate with an oscillation frequency of more than 340 kHz, corresponding to a propagation delay of less than 210 nanoseconds per stage.

High-Field-Effect Mobility of Low-Crystallinity Conjugated Polymers with Localized Aggregates.

Charge carriers typically move faster in crystalline regions than in amorphous regions in conjugated polymers because polymer chains adopt a regular arrangement resulting in a high degree of π-π stacking in crystalline regions. In contrast, the random polymer chain orientation in amorphous regions hinders connectivity between conjugated backbones; thus, it hinders charge carrier delocalization. Various studies have attempted to enhance charge carrier transport by increasing crystallinity. However, these approaches are inevitably limited by the semicrystalline nature of conjugated polymers. Moreover, high-crystallinity conjugated polymers have proven inadequate for soft electronics applications because of their poor mechanical resilience. Increasing the polymer chain connectivity by forming localized aggregates via π-orbital overlap among several conjugated backbones in amorphous regions provides a more effective approach to efficient charge carrier transport. A simple strategy relying on the density of random copolymer alkyl side chains was developed to generate these localized aggregates. In this strategy, steric hindrance caused by these side chains was modulated to change their density. Interestingly, a random polymer exhibiting low alkyl side chain density and crystallinity displayed greatly enhanced field-effect mobility (1.37 cm(2)/(V·s)) compared with highly crystalline poly(3-hexylthiophene).

Synthesis of ultrathin polymer insulating layers by initiated chemical vapour deposition for low-power soft electronics.

Insulating layers based on oxides and nitrides provide high capacitance, low leakage, high breakdown field and resistance to electrical stresses when used in electronic devices based on rigid substrates. However, their typically high process temperatures and brittleness make it difficult to achieve similar performance in flexible or organic electronics. Here, we show that poly(1,3,5-trimethyl-1,3,5-trivinyl cyclotrisiloxane) (pV3D3) prepared via a one-step, solvent-free technique called initiated chemical vapour deposition (iCVD) is a versatile polymeric insulating layer that meets a wide range of requirements for next-generation electronic devices. Highly uniform and pure ultrathin films of pV3D3 with excellent insulating properties, a large energy gap (>8 eV), tunnelling-limited leakage characteristics and resistance to a tensile strain of up to 4% are demonstrated. The low process temperature, surface-growth character, and solvent-free nature of the iCVD process enable pV3D3 to be grown conformally on plastic substrates to yield flexible field-effect transistors as well as on a variety of channel layers, including organics, oxides, and graphene.

An improvement of performance in n-channel organic field effect transistors with N-phenyl[60]fulleropyrrolidines by molecular doping.

The high performance of soluble [60]fulleropyrrolidine upon its use as the active layer of n-channel organic field-effect transistors (OFETs) is reported. The two materials, N-phenyl derivatives C60-fused-N-phenyl-2-phenylpyrrolidine ([C60]PhNPh) and C60-fused N-phenyl-2-hexylpyrrolidine ([C60]HexNPh), have well-controlled molecular structures with a modification of the pyrrolidine ring, with no increase in the LUMO level, achieving a high mobility and highly ambient stable n-type OFET. The top-gate, bottom-contact device shows a high electron charge-carrier mobility of up to 0.14 and 0.08 cm(2) V(-1) s(-1) for [C60]PhNPh and [C60]HexNPh, respectively, (Ion/Ioff = 10(6)) with the commonly used CYTOP dielectric. Excess carriers introduced by a small amount of chemical doping of polyethyleneimine (PEI) compensate traps by shifting the Fermi level (EF) toward the respective transport energy levels and therefore increase charge-carrier mobility (0.26 and 0.1 cm(2) V(-1) s(-1)) and provide good ambient operational stability compared with pristine devices.

Improved electron transport properties of n-type naphthalenediimide polymers through refined molecular ordering and orientation induced by processing solvents.

To determine the role played by the choice of processing solvents in governing the photophysics, microstructure, and charge carrier transport in naphthalenediimide (NDI)-based polymers, we have prepared two new NDI-bithiophene (T2)- and NDI-thienothiophene (TTh)-containing polymers with hybrid siloxane pentyl chains (SiC5) (P(NDI2SiC5-T2) and P(NDI2SiC5-TTh)). Among the various processing solvents studied here, the films prepared using chloroform exhibited far better electron mobilities (0.16 ± 0.1-0.21 ± 0.05 cm(2) V(-1) s(-1)) than the corresponding samples prepared from different solvents, exceeding one order of magnitude higher, indicating the significant influence of the processing solvent on the charge transport. Upon thin-film analysis using atomic force microscopy and grazing incidence X-ray diffraction, we discovered that molecular ordering and orientation are affected by the choice of the processing solvent, which is responsible for the change in the transport characteristics of this class of polymers.

Charge transport dependent high open circuit voltage tandem organic photovoltaic cells with low temperature deposited HATCN-based charge recombination layers.

Mechanisms of charge transport between the interconnector and its neighboring layers in tandem organic photovoltaic cells have been systematically investigated by studying electronic properties of the involving interfaces with photoelectron spectroscopies and performance of the corresponding devices. The results show that charge recombination occurs at HATCN and its neighboring hole transport layers which can be deposited at low temperature. The hole transport layer plays an equal role to the interconnector itself. These insights provide guidance for the identification of new materials and the device architecture for high performance devices.

Development of high-performance printed organic field-effect transistors and integrated circuits.

Organic electronics is regarded as an important branch of future microelectronics especially suited for large-area, flexible, transparent, and green devices, with their low cost being a key benefit. Organic field-effect transistors (OFETs), the primary building blocks of numerous expected applications, have been intensively studied, and considerable progress has recently been made. However, there are still a number of challenges to the realization of high-performance OFETs and integrated circuits (ICs) using printing technologies. Therefore, in this perspective article, we investigate the main issues concerning developing high-performance printed OFETs and ICs and seek strategies for further improvement. Unlike many other studies in the literature that deal with organic semiconductors (OSCs), printing technology, and device physics, our study commences with a detailed examination of OFET performance parameters (e.g., carrier mobility, threshold voltage, and contact resistance) by which the related challenges and potential solutions to performance development are inspected. While keeping this complete understanding of device performance in mind, we check the printed OFETs' components one by one and explore the possibility of performance improvement regarding device physics, material engineering, processing procedure, and printing technology. Finally, we analyze the performance of various organic ICs and discuss ways to optimize OFET characteristics and thus develop high-performance printed ICs for broad practical applications.

Controlling charge injection properties in polymer field-effect transistors by incorporation of solution processed molybdenum trioxide.

A simply and facilely synthesized MoO3 solution was developed to fabricate charge injection layers for improving the charge-injection properties in p-type organic field-effect transistors (OFETs). By dissolving MoO3 powder in ammonium (NH3) solvent under an air atmosphere, an intermediate ammonium molybdate ((NH4)2MoO4) precursor is made stable, transparent and spin-coated to form the MoO3 interfacial layers, the thickness and morphology of which can be well-controlled. When the MoO3 layer was applied to OFETs with a cost-effective molybdenum (Mo) electrode, the field-effect mobility (µFET) was significantly improved to 0.17 or 1.85 cm(2) V(-1)s(-1) for polymer semiconductors, regioregular poly(3-hexylthiophene) (P3HT) or 3,6-bis-(5bromo-thiophen-2-yl)-N,N'-bis(2-octyl-1-dodecyl)-1,4-dioxo-pyrrolo[3,4-c]pyrrole (DPPT-TT), respectively. Device analysis indicates that the MoO3-deposited Mo contact exhibits a contact resistance RC of 1.2 MΩ cm comparable to that in a device with the noble Au electrode. Kelvin-probe measurements show that the work function of the Mo electrode did not exhibit a dependence on the thickness of MoO3 film. Instead, ultraviolet photoemission spectroscopy results show that a doping effect is probably induced by casting the MoO3 layer on the P3HT semiconductor, which leads to the improved hole injection.

A thienoisoindigo-naphthalene polymer with ultrahigh mobility of 14.4 cm(2)/V·s that substantially exceeds benchmark values for amorphous silicon semiconductors.

By considering the qualitative benefits associated with solution rheology and mechanical properties of polymer semiconductors, it is expected that polymer-based electronic devices will soon enter our daily lives as indispensable elements in a myriad of flexible and ultra low-cost flat panel displays. Despite more than a decade of research focused on designing and synthesizing state-of-the-art polymer semiconductors for improving charge transport characteristics, the current mobility values are still not sufficient for many practical applications. The confident mobility in excess of ∼10 cm(2)/V·s is the most important requirement for enabling the realization of the aforementioned near-future products. We report on an easily attainable donor-acceptor (D-A) polymer semiconductor: poly(thienoisoindigo-alt-naphthalene) (PTIIG-Np). An unprecedented mobility of 14.4 cm(2)/V·s, by using PTIIG-Np with a high-k gate dielectric poly(vinylidenefluoride-trifluoroethylene) (P(VDF-TrFE)), is achieved from a simple coating processing, which is of a magnitude that is very difficult to obtain with conventional TFTs by means of molecular engineering. This work, therefore, represents a major step toward truly viable plastic electronics.

Organic field-effect transistors by a solvent vapor annealing process.

Organic field-effect transistor (OFET) attracts great interests from scientific research and industrial application because of its low-cost fabrication and excellent mechanical flexibility. Yet the charge carrier mobility of typical OFET is still around 1-5 cm2/Vs and needs to be further enhanced, ideally by cost effective processes or treatments. Here we review one of the straightforward but effective methods, solvent vapor annealing (SVA), to improve the crystallinity of organic semiconductor film leading enhancement of charge carrier mobility in OFETs. We start by introducing the basic mechanism of SVA, followed by experimental works on small molecules and then conjugated polymers. Along with those examples, we discuss the important factors in using SVA to form highly crystalline conjugated molecule films or organic single crystals to achieve high performance OFETs.

Alkylated fullerene derivatives for solution-processable organic thin-film transistors and bulkheterojunction solar cells.

In this paper, we report synthesis and characterization of alkylated fullerene derivatives for solution-processable organic thin film transistors and solar cells. Their physical, thermal, and semiconducting properties have been studied. Organic thin-film transistors fabricated from C60TH-Oc exhibit electron mobilities as high as 3.2 x 10(-2) cm2 V(-1) s(-1) with 32 V of a threshold voltage. The best power conversion efficiency (PCE) was observed in a layered structure P3HT:C60TH-Oc (PCE = 0.44%), which was a twice value of P3HT:C60TH-Dd (PCE = 0.23%).

Boosting the Performance of Photomultiplication-Type Organic Photodiodes by Embedding CsPbBr3 Perovskite Nanocrystals.

In this study, it is demonstrated that CsPbBr3 perovskite nanocrystals (NCs) can enhance the overall performances of photomultiplication-type organic photodiodes (PM-OPDs). The proposed approach enables the ionic-polarizable CsPbBr3 NCs to be evenly distributed throughout the depletion region of Schottky junction interface, allowing the entire trapped electrons within the depletion region to be stabilized, in contrast to previously reported interface-limited strategies. The optimized CsPbBr3 -NC-embedded poly(3-hexylthiophene-diyl)-based PM-OPDs exhibit exceptionally high external quantum efficiency, specific detectivity, and gain-bandwidth product of 2,840,000%, 3.97 × 1015 Jones, and 2.14 × 107  Hz, respectively. 2D grazing-incidence X-ray diffraction analyses and drift-diffusion simulations combined with temperature-dependent J-V characteristic analyses are conducted to investigate the physics behind the success of CsPbBr3 -NC-embedded PM-OPDs. The results show that the electrostatic interactions generated by the ionic polarization of NCs effectively stabilize the trapped electrons throughout the entire volume of the photoactive layer, thereby successfully increasing the effective energy depth of the trap states and allowing efficient PM mechanisms. This study demonstrates how a hybrid-photoactive-layer approach can further enhance PM-OPD when the functionality of inorganic inclusions meets the requirements of the target device.

Two-Dimensional Tunneling Memtransistor with Thin-Film Heterostructure for Low-Power Logic-in-Memory Complementary Metal-Oxide Semiconductor.

With the demand for high-performance and miniaturized semiconductor devices continuously rising, the development of innovative tunneling transistors via efficient stacking methods using two-dimensional (2D) building blocks has paramount importance in the electronic industry. Hence, 2D semiconductors with atomically thin geometries hold significant promise for advancements in electronics. In this study, we introduced tunneling memtransistors with a thin-film heterostructure composed of 2D semiconducting MoS2 and WSe2. Devices with the dual function of tuning and memory operation were realized by the gate-regulated modulation of the barrier height at the heterojunction and manipulation of intrinsic defects within the exfoliated nanoflakes using solution processes. Further, our investigation revealed extensive edge defects and four distinct defect types, namely monoselenium vacancies, diselenium vacancies, tungsten vacancies, and tungsten adatoms, in the interior of electrochemically exfoliated WSe2 nanoflakes. Additionally, we constructed complementary metal-oxide semiconductor-based logic-in-memory devices with a small static power in the range of picowatts using the developed tunneling memtransistors, demonstrating a promising approach for next-generation low-power nanoelectronics.

All-Solution-Processed High-Performance MoS2 Thin-Film Transistors with a Quasi-2D Perovskite Oxide Dielectric.

Assembling solution-processed van der Waals (vdW) materials into thin films holds great promise for constructing large-scale, high-performance thin-film electronics, especially at low temperatures. While transition metal dichalcogenide thin films assembled in solution have shown potential as channel materials, fully solution-processed vdW electronics have not been achieved due to the absence of suitable dielectric materials and high-temperature processing. In this work, we report on all-solution-processedvdW thin-film transistors (TFTs) comprising molybdenum disulfides (MoS2) as the channel and Dion-Jacobson-phase perovskite oxides as the high-permittivity dielectric. The constituent layers are prepared as colloidal solutions through electrochemical exfoliation of bulk crystals, followed by sequential assembly into a semiconductor/dielectric heterostructure for TFT construction. Notably, all fabrication processes are carried out at temperatures below 250 °C. The fabricated MoS2 TFTs exhibit excellent device characteristics, including high mobility (>10 cm2 V-1 s-1) and an on/off ratio exceeding 106. Additionally, the use of a high-k dielectric allows for operation at low voltage (∼5 V) and leakage current (∼10-11 A), enabling low power consumption. Our demonstration of the low-temperature fabrication of high-performance TFTs presents a cost-effective and scalable approach for heterointegrated thin-film electronics.

Synthesis of poly(p-phenylene-vinylene) derivatives containing an oxadiazole pendant group and their applications to organic electronic devices.

Poly(p-phenylene vinylene) (PPV) derivatives with 2,5-diphenyl-1,3,4-oxadiazole-diyl (OXD) as the side chain, poly[2-{4-[5-(4-(heptyloxy)phenyl)-1,3,4-oxadiazole-2-yI]phenyl-oxy}-1,4-phenylene-vinylene] (OXH-PPV), poly[2-{4-[5-(4-(heptyloxy)phenyl)-1,3,4-oxadia-zole-2-yl]phenyl-oxy}-1,4-phenylenevinylene-co-2-methoxy-5-(2'-ethylhexyloxy)-p-phenylene vinylene] (OXH-PPV-co-MEH-PPV), and poly[2-methoxy-5-(2'-ethylhexyl-oxy)-p-phenylene vinylene] (MEH-PPV), were synthesized via a modified Gilch route. The electron-deficient oxadiazole moiety was introduced on the side chain of the polymer backbone to increase the electron-affinity of the polymers. The electroluminescent (EL) properties of the resulting polymers as an active layer, were investigated by the fabrication of single-layer LEDs and the devices using OXH-PPV-co-MEH-PPV showed better EL properties than those using pure MEH-PPV. Also, to investigate the switching properties of the resulting polymers as an active layer, OFET devices were fabricated in a top-contact/bottom-gate configuration. The resulting FETs exhibited typical p-channel characteristics, field-effect mobility of 6.5 x 10(-4) - 7.0 x 10(-5) cm2 V(-1) s(-1), and on-off ratio of about 10(4)-10(5).

Large Transconductance of Electrochemical Transistors Based on Fluorinated Donor-Acceptor Conjugated Polymers.

Organic electrochemical transistors (OECTs) have enormous potential for use in biosignal amplifiers, analyte sensors, and neuromorphic electronics owing to their exceptionally large transconductance. However, it is challenging to simultaneously achieve high charge carrier mobility and volumetric capacitance, the two most important figures of merit in OECTs. Herein, a method of achieving high-performance OECT with donor-acceptor conjugated copolymers by introducing fluorine units is proposed. A series of cyclopentadithiophene-benzothiadiazole (CDT-BT) copolymers for use in high-performance OECTs with enhanced charge carrier mobility (from 0.65 to 1.73 cm2·V-1·s-1) and extended volumetric capacitance (from 44.8 to 57.6 F·cm-3) by fluorine substitution is achieved. The increase in the volumetric capacitance of the fluorinated polymers is attributed to either an increase in the volume at which ions can enter the film or a decrease in the effective distance between the ions and polymer backbones. The fluorine substitution increases the backbone planarity of the CDT-BT copolymers, enabling more efficient charge carrier transport. The fluorination strategy of this work suggests the more versatile use of conjugated polymers for high-performance OECTs.