Single-Component CMOS-Like Logic using Diketopyrrolopyrrole-Based Ambipolar Organic Electrochemical Transistors

Complementary circuits based on organic electrochemical transistors (OECTs) are attractive for the development of inexpensive and disposable point-of-care bioelectronic devices. Ambipolar OECTs, which employ a single channel material, could decrease the fabrication complexity and manufacturing costs of such circuits. An ideal channel material for ambipolar OECTs should be electrochemically stable in aqueous environments, afford facile ion insertion for both cations and anions, and also facilitate high and balanced electron and hole transport. In this study, triethylene glycol functionalized diketopyrrolopyrrole (DPP)-based polymer is proposed for the development of ambipolar OECTs. It is shown that DPP-based OECTs have a high and comparable figure of merit for both n- and p-type operations. Logic NOT, NAND, and NOR operations with corresponding complementary circuits constructed from identical DPP-based OECT devices are demonstrated. This study is an important step toward the development of sophisticated complementary metal–oxide–semiconductor-like logic circuits using single-component OECTs.     

Analog Circuit Applications Based on All‐2D Ambipolar ReSe2 Field‐Effect Transistors

Complementary circuits based on 2D materials show great promise for next‐generation electronics. An ambipolar all‐2D ReSe₂ field‐effect transistor (FET) with a hexagonal boron nitride gate dielectric is fabricated and its electronic characteristics are comprehensively studied by temperature dependence and noise measurements. Ambipolar transfer characteristics are achieved owing to the tunable Fermi level of the graphene contact and negligible and 30 meV Schottky barrier heights for the n‐ and p‐channel regimes, respectively. An inverter is also fabricated to demonstrate ambipolar ReSe₂ FET operation in a logic circuit. Furthermore, a p/n switchable unipolar FET is designed and shows potential for building complimentary circuits from a signal device. This work demonstrates the potential of all‐2D ReSe₂ FETs and makes available new approaches for designing next‐generation devices.     

Novel Photoinduced Recovery of OFET Memories Based on Ambipolar Polymer Electret for Photorecorder Application

A new design concept for novel photoresponsive flash organic field‐effect transistor (OFET) memory is demonstrated by employing the carbazoledioxazine polymer (Poly CD) as an electret. Photoactive electrets that can absorb the light effectively rather than photoactive semiconductors are proposed by the “photoinduced recovery” mechanism in the literature; however, the correlation between the chemical structure and photoresponsive electrical performances is ambiguous. In this study, it is reported for the first time that the OFET memory with trapped charges can be optically recovered by a polymer electret and the working mechanism can be explained by the structural design. The highly planar Poly CD electret exhibits photoluminescence quenching in film states, resulting in the generation of sufficient excitons to eliminate trapped charges under light excitation. Additionally, the Poly CD electret with coplanar donor–acceptor moieties is suitable for both p‐channel and n‐channel semiconductors. For p‐type memory devices, a large memory window (82 V) and stable nonvolatile retention performance with high ON/OFF ratio could be obtained. The memories also display good switching reliability for voltage‐programming and light‐erasing cycles. This study provides useful information for the development of polymer‐based photoresponsive flash OFET memories and demonstrates the practical applications of photorecorder and photosensitive smart tag.     

Solution‐Deposited Zinc Oxide and Zinc Oxide/Pentacene Bilayer Transistors: High Mobility n‐Channel,Ambipolar, and Nonvolatile Devices

A solution processed n‐channel zinc oxide (ZnO) field effect transistor (FET) was fabricated by simple dip coating and subsequent heat treatment of a zinc acetate film. The field effect mobility of electrons depends on ZnO grain size, controlled by changing the number of coatings and zinc acetate solution concentration. The highest electron mobility achieved by this method is 7.2 cm² V^?1 s^?1 with On/Off ratio of 70. This electron mobility is higher than for the most recently reported solution processed ZnO transistor. We also fabricated bilayer transistors where the first layer is ZnO, and the second layer is pentacene, a p‐channel organic which is deposited by thermal evaporation. By changing the ZnO grain size (or thickness) this type of bilayer transistor shows p‐channel, ambipolar and n‐channel behavior. For the ambipolar transistor, well balanced electron and hole mobilities are 7.6 × 10^?3 and 6.3 × 10^?3 cm² V^?1 s^?1 respectively. When the ZnO layer is very thin, the transistor shows p‐channel behavior with very high reversible hysteresis. The nonvolatile tuning function of this transistor was investigated.     

Controlling Ambipolar Charge Transport in Isoindigo‐Based Conjugated Polymers by Altering Fluorine Substitution Position for High‐Performance Organic Field‐Effect Transistors

A molecular design strategy to achieve highly balanced ambipolar charge transport for donor–acceptor (D–A) isoindigo (IIG)‐based copolymer through systematic selection of fluorination positions is reported. To study fluorine substitution site effects on electronic and structural properties, two fluorinated IIG‐based copolymers (PIIG‐iFT2 and PIIG‐oFT2) are synthesized, which contain two fluorine atoms at the bithiophene (T2) inner and outer site and compare them with a nonfluorinated copolymer of IIG and T2 (PIIG‐T2) as the reference polymer. Fluorination at the outer site of T2 in PIIG‐oFT2 polymer effectively lowers molecular energy levels and increases molecular planarity more than fluorination at the T2 inner site. PIIG‐oFT2 organic field‐effect transistors show highly balanced ambipolar mobility, hole mobility (μ_h)/electron mobility (μ_e) = 1 by increasing electron mobility, whereas PIIG‐T2 (μ_h/μ_e = 9.0) and PIIG‐iFT2 (μ_h/μ_e = 2.4) exhibit unbalanced ambipolar transport. The ambipolar complementary‐like inverter is also demonstrated by simple one‐time coating of PIIG‐oFT2 with gain = 21.     

Reconfigurable Multifunctional Ambipolar Polymer-Blend Transistors with Improved Switching-Off Capability

Ambipolar field-effect transistors allowing both holes and electrons transport can work in different states, which are attractive for simplifying the manufacture of circuits and endowing the circuits with reconfigurable multi-functionalities. However, conventional ambipolar transistors intrinsically suffer from poor switching-off capability because the gate electrode is not able to simultaneously deplete holes and electrons across the entire transport channel, which hurdles the practical applications. This study shows that the switching-off capability of polymer ambipolar transistor is significantly improved by up to three orders by introducing non-uniformly distributed compensation potentials along the channel to synchronically tune the charge transport at different channel locations. The non-uniform compensation potential is experimentally generated by the non-uniformly distributed electret charges, which are pre-injected into the insulators from source and drain electrodes. By this method, both n-type and p-type operations with high mobility (2.2 and 0.8 cm²s⁻¹V⁻¹ respectively) and high on/off ratio (10⁵) are obtained in the same device, and the different states are reversibly switchable. Moreover, this method endows the device with diverse device characteristics and reconfigurable multi-functionalities, which promotes the application of ambipolar transistors in complementary metal-oxide semiconductors-like circuits and some emerging electronics, including reconfigurable devices, multi-level memories, and artificial synapses.     

Phototuning Selectively Hole and Electron Transport in Optically Switchable Ambipolar Transistors

One of the grand challenges in organic electronics is to develop multicomponent materials wherein each component imparts a different and independently addressable property to the hybrid system. In this way, the combination of the pristine properties of each component is not only preserved but also combined with unprecedented properties emerging from the mutual interaction between the components. Here for the first time, that tri‐component materials comprised of an ambipolar diketopyrrolopyrrole‐based semiconducting polymer combined with two different photochromic diarylethene molecules possessing ad hoc energy levels can be used to develop organic field‐effect transistors, in which the transport of both, holes and electrons, can be photo‐modulated. A fully reversible light‐switching process is demonstrated, with a light‐controlled 100‐fold modulation of p‐type charge transport and a tenfold modulation of n‐type charge transport. These findings pave the way for photo‐tunable inverters and ultimately for completely re‐addressable high‐performance circuits comprising optical storage units and ambipolar field‐effect transistors.     

Selectively Fluorinated Furan-Phenylene Co-Oligomers Pave the Way to Bright Ambipolar Light-Emitting Electronic Devices

Linearly conjugated oligomers attract ever-growing attention as promising systems for organic optoelectronics because of their inherent lucky combination of high charge mobility and bright luminescence. Among them, furan-phenylene co-oligomers (FPCOs) are distinguished by outstanding solubility, very bright luminescence, and good hole-transport properties; however, furan-containing organic semiconductors generally lack electron transport, which makes it impossible to utilize them in efficient light-emitting electronic devices, specifically, ambipolar light-emitting transistors. In this work, 1,4-bis(5-phenylfuran-2-yl)benzene (FP5) derivatives are synthesized with the fully/partially fluorinated central and edge phenyl rings. It is shown that the selective fluorination of FPCOs lowers the energies of frontier molecular orbitals, maintaining the bandgap, solubility, and bright luminescence, dramatically improves the photostability, tunes the π-π stacked packing, and allows the first realization of electron transport in FPCOs. It is found that selectively fluorinated 2,2′-(2,3,5,6-tetrafluoro-1,4-phenylene)bis[5-(3,5-difluorophenyl)furan] demonstrates well-balanced ambipolar charge transport and efficient electroluminescence in an organic light-emitting transistor (OLET) with external quantum and luminous efficiencies as high as 0.63% and 5 cdA⁻¹, respectively, which are among the best reported for OLETs. The findings show that “smart” fluorination is a powerful tool to fine-tune the stability and performance of linearly conjugated small molecules for organic optoelectronics.     

Flexible,Conformal Organic Synaptic Transistors on Elastomer for Biomedical Applications

Bioelectronics in synaptic transistors for future biomedical applications, such as implanted treatments and human–machine interfaces, must be flexible with good mechanical compatibility with biological tissues. The rigid nature and high deposition temperature in conventional inorganic synaptic transistors restrict the development of flexible, conformal synaptic devices. Here, the dinaphtho[2,3‐b:2′,3′‐f]thieno[3,2‐b]‐thiophene organic synaptic transistor on elastic polydimethylsiloxane is demonstrated to avoid these limitations. The unique advantages of organic materials in low Young's modulus and low temperature process enable seamless adherence of organic synaptic transistors on arbitrary‐shaped objects. On 3D curved surfaces, the essential synaptic functions, such as potentiation/depression, short/long‐term synaptic plasticity, and spike voltage–dependent plasticity, are successfully realized. The time‐dependent surface potential characterization reveals the slow polarization of dipoles in the dielectric is responsible for hysteresis and synaptic behaviors. This work represents that organic materials offer a potential platform to realize the flexible, conformal synaptic transistors for the development of wearable and implantable artificial neuromorphic systems.     

有机场效应晶体管最新实验研究进展

介绍了近两年新报道的有机半导体材料,列举了其场效应性能参数;综述了有机场效应晶体管(OFET)在器件结构上的改进,重点阐述了基于常见有机功能层材料富勒烯及其衍生物、并五苯、聚3-己基噻吩的OFET对栅介质层及有机功能层与电极的界面的改进,讨论了器件结构改进对OFET阈值电压、开关比、载流子迁移率的影响;介绍了衬底温度、退火处理对OF-ET性能的影响。最后,针对有机场效应晶体管研究现状,指出未来研究中应注重开发高迁移率、高薄膜稳定性的有机功能材料和高介电常数、高成膜质量的有机栅介质材料,继续优化器件结构,改进制备工艺以提高器件性能。     

Carbon Nanotube Based Multifunctional Ambipolar Transistors for AC Applications

Field‐effect transistors (FETs) fabricated on large diameter carbon nanotubes (CNTs) present typical ambipolar transfer characteristics owing to the small band‐gap of CNTs. Depending on the DC biasing condition, the ambipolar FET can work in three different regions, and then can be used as the core to realize multifunctional AC circuits. The CNT FET based circuits can work as a high‐efficiency ambipolar frequency doubler in the ambipolar transfer region, and also can function as in‐phase amplifier and inverted amplifier in the linear transfer region. Due to current saturation of the CNT FET, an AC amplifier with a voltage gain of 2 is realized when the device works in the linear transfer region. Achieving an actual amplification and frequency doubling functions indicates that complicated radio frequency circuits or systems can be constructed based on just one kind of device: ambipolar CNT FETs.     

Heterojunction Ambipolar Organic Transistors Fabricated by a Two‐Step Vacuum‐Deposition Process

Ambipolar organic field‐effect transistors (OFETs) are produced, based on organic heterojunctions fabricated by a two‐step vacuum‐deposition process. Copper phthalocyanine (CuPc) deposited at a high temperature (250 °C) acts as the first (p‐type component) layer, and hexadecafluorophthalocyaninatocopper (F₁₆CuPc) deposited at room temperature (25 °C) acts as the second (n‐type component) layer. A heterojunction with an interpenetrating network is obtained as the active layer for the OFETs. These heterojunction devices display significant ambipolar charge transport with symmetric electron and hole mobilities of the order of 10^–4 cm² V^–1 s^–1 in air. Conductive channels are at the interface between the F₁₆CuPc and CuPc domains in the interpenetrating networks. Electrons are transported in the F₁₆CuPc regions, and holes in the CuPc regions. The molecular arrangement in the heterojunction is well ordered, resulting in a balance of the two carrier densities responsible for the ambipolar electrical characteristics. The thin‐film morphology of the organic heterojunction with its interpenetrating network structure can be controlled well by the vacuum‐deposition process. The structure of interpenetrating networks is similar to that of the bulk heterojunction used in organic photovoltaic cells, therefore, it may be helpful in understanding the process of charge collection in organic photovoltaic cells.     

Recent Developments and Novel Applications of Thin Film,Light‐Emitting Transistors

Light‐emitting field‐effect transistors (LEFETs) combine switching and amplification with light emission and thus represent an interesting optoelectronic device. They are not limited anymore to a few examples and specific materials but are nearly universal for a wide range of semiconductors, from organic to inorganic and nanoscale. This review introduces the basic working principles of lateral unipolar and ambipolar LEFETs and discusses recent examples based on various solution‐processed semiconducting materials. Applications beyond simple light emission are presented and possible future directions for light‐emitting transistors with added functionalities are outlined.     

Recent Advances in the Bias Stress Stability of Organic Transistors

In this progress report, recent advances in the development of organic transistors with superior bias stress stability and in the understanding of the charge traps that degrade device performance under prolonged bias stress are reviewed, with a particular focus on materials science and engineering methods. The phenomenological aspects of bias stress effects and the experimental methods for investigating charge traps are described. The recent progress in the bias stress stability of organic transistors is discussed in terms of those components that are the main focus of attempts to improve bias stress stability, i.e., organic semiconductor layers, gate dielectrics, and source/drain contacts. A brief summary of this progress is presented and the outlook for future research in this field is assessed. This report aims to summarize recent progress in this field and to provide some guidelines for studying bias stress–induced charge‐trapping phenomena.     

Pressure‐Tunable Ambipolar Conduction and Hysteresis in Thin Palladium Diselenide Field Effect Transistors

Few‐layer palladium diselenide (PdSe₂) field effect transistors are studied under external stimuli such as electrical and optical fields, electron irradiation, and gas pressure. The ambipolar conduction and hysteresis are observed in the transfer curves of the as‐exfoliated and unprotected PdSe₂ material. The ambipolar conduction and its hysteretic behavior in the air and pure nitrogen environments are tuned. The prevailing p‐type transport observed at atmospheric pressure is reversibly turned into a dominant n‐type conduction by reducing the pressure, which can simultaneously suppress the hysteresis. The pressure control can be exploited to symmetrize and stabilize the transfer characteristics of the device as required in high‐performance logic circuits. The transistors are affected by trap states with characteristic times in the order of minutes. The channel conductance, dramatically reduced by the electron irradiation during scanning electron microscope imaging, is restored after an annealing of several minutes at room temperature. The work paves the way toward the exploitation of PdSe₂ in electronic devices by providing an experiment‐based and deep understanding of charge transport in PdSe₂ transistors subjected to electrical stress and other external agents.     

Half‐Fused Diketopyrrolopyrrole‐Based Conjugated Donor–Acceptor Polymer for Ambipolar Field‐Effect Transistors

A novel building block, denoted as half‐fused diketopyrrolopyrrole (DPP) (9‐(3‐octadecylhenicosyl)‐8‐(thiophen‐2‐yl)‐7H‐pyrrolo[3,4‐a]thieno[3,2‐g]indolizine‐7,10(9H)‐dione), in which one of the flanking thiophene units is fused to one of the DPP rings via a carbon‐carbon double bond at the N‐position is reported. The half‐fused DPP is successfully utilized as an electron acceptor to prepare the conjugated donor–acceptor polymer PTFDFT , which exhibits ambipolar semiconducting behavior in ambient air. Theoretical calculations and absorption spectral studies show that the backbone of PTFDFT is more planar compared to the reference polymer with conventional DPP units. As a result, PTFDFT shows a narrow bandgap and low lowest unoccupied molecular orbital level. The more planar backbone with fewer side chains favors the dense packing of the polymer chains of PTFDFT with a short π–π stacking distance (3.49 Å). Grazing‐incidence wide‐angle X‐ray scattering data further confirm the predominant edge‐on packing mode of the PTFDFT polymer chains on the substrate. As expected, the PTFDFT thin film shows excellent ambipolar semiconducting properties under ambient conditions, reaching 2.23 and 1.08 cm² V^?1 s^?1 for the n‐ and p‐channels, respectively. In addition, complementary‐like inverter with gain value as high as 141 is successfully constructed using the PTFDFT thin film.     

MXene Electrode for the Integration of WSe2 and MoS2 Field Effect Transistors

Recently, MXenes, which are 2D early transition metal carbides and carbonitrides, have attracted wide attention because of their excellent conductivities. Here, the electrode applications of Ti₂C(OH)_xF_y, one member of the MXene family, in WSe₂ and MoS₂ field effect transistors (FETs) are assessed. Kelvin probe force microscopy analysis is performed to determine its work function, which is estimated to be ≈4.98 eV. Devices based on WSe₂/Ti₂C(OH)_xF_y and MoS₂/Ti₂C(OH)_xF_y heterostructures are fabricated with the mechanical transfer method and their electronic performances evaluated. The temperature‐dependent current–voltage transfer characteristics of the devices are determined to extract their Schottky barrier heights. The hole barrier between WSe₂ and Ti₂C(OH)_xF_y is estimated to be ≈0.23 eV and the electron barrier between the MoS₂ band and Ti₂C(OH)_xF_y is ≈0.19 eV, which indicates that the pinning effect occurs at the MoS₂/Ti₂C(OH)_xF_y interface but not at the WSe₂/Ti₂C(OH)_xF_y interface; this difference arises because of the difference between the band structures of WSe₂ and MoS₂. A complementary metal–oxide–semiconductor inverter based on these electrode properties of Ti₂C(OH)_xF_y with MoS₂ (n‐channel) and WSe₂ (p‐channel) is fabricated, which demonstrates that Ti₂C(OH)_xF_y is a promising electrode for future nanoelectronics applications.     

Understanding,Optimizing, and Utilizing Nonideal Transistors Based on Organic or Organic Hybrid Semiconductors

Many advanced materials have been developed for organic field‐effect transistors (OFETs) or thin‐film transistors (TFTs) based on organic and organic hybrid materials. However, although many new OFETs exhibit superior characteristic parameters (such as high mobility), most of them show nonideal performances that have strongly limited progress in the design of molecules, the understanding of transport mechanisms, and the circuit applications of OFETs. In this review, the device physics of ideal and nonideal OFETs is discussed first to understand the factors that limit effective mobility in semiconducting channels, distort the potential distribution, or reduce the drift electric field. Then, recent advances in optimizing the material combinations, device structures, and fabrications of OFETs toward ideal transistors are discussed. Based on the good control of materials and interfaces, some new and novel concepts to utilize the nonideal properties of OFETs to build low‐power circuits and integrated sensors are also discussed.