Device design principles and bioelectronic applications for flexible organic electrochemical transistors

Organic electrochemical transistors(OECTs) exhibit significant potential for applications in healthcare and human-machine interfaces, due to their tunable synthesis, facile deposition, and excellent biocompatibility. Expanding OECTs to the fexible devices will significantly facilitate stable contact with the skin and enable more possible bioelectronic applications. In this work,we summarize the device physics of fexible OECTs, aiming to offer a foundational understanding and guidelines for material selection and device architecture. Particular attention is paid to the advanced manufacturing approaches, including photolithography and printing techniques, which establish a robust foundation for the commercialization and large-scale fabrication. And abundantly demonstrated examples ranging from biosensors, artificial synapses/neurons, to bioinspired nervous systems are summarized to highlight the considerable prospects of smart healthcare. In the end, the challenges and opportunities are proposed for fexible OECTs. The purpose of this review is not only to elaborate on the basic design principles of fexible OECTs, but also to act as a roadmap for further exploration of wearable OECTs in advanced bio-applications.

Transient Response and Ionic Dynamics in Organic Electrochemical Transistors

The rapid development of organic electrochemical transistors(OECTs)has ushered in a new era in organic electronics,distinguishing itself through its application in a variety of domains,from high-speed logic circuits to sensitive biosensors,and neuromorphic devices like artificial synapses and organic electrochemical random-access memories.Despite recent strides in enhancing OECT performance,driven by the demand for superior transient response capabilities,a comprehensive understanding of the complex interplay between charge and ion transport,alongside electron–ion interactions,as well as the optimization strategies,remains elusive.This review aims to bridge this gap by providing a systematic overview on the fundamental working principles of OECT transient responses,emphasizing advancements in device physics and optimization approaches.We review the critical aspect of transient ion dynamics in both volatile and non-volatile applications,as well as the impact of materials,morphology,device structure strategies on optimizing transient responses.This paper not only offers a detailed overview of the current state of the art,but also identifies promising avenues for future research,aiming to drive future performance advancements in diversified applications.

Recent advances in fabrication and functions of neuromorphic system based on organic field effect transistor

The development of various artificial electronics and machines would explosively increase the amount of information and data,which need to be processed via in-situ remediation.Bioinspired synapse devices can store and process signals in a parallel way,thus improving fault tolerance and decreasing the power consumption of artificial systems.The organic field effect transistor(OFET)is a promising component for bioinspired neuromorphic systems because it is suitable for large-scale integrated circuits and flexible devices.In this review,the organic semiconductor materials,structures and fabrication,and different artificial sensory perception systems functions based on neuromorphic OFET devices are summarized.Subsequently,a summary and challenges of neuromorphic OFET devices are provided.This review presents a detailed introduction to the recent progress of neuromorphic OFET devices from semiconductor materials to perception systems,which would serve as a reference for the development of neuromorphic systems in future bioinspired electronics.

Grain boundary engineering of organic semiconductor films in organic transistors

Organicfield-effect transistors(OFETs)show great application potential in organic electronic and optoelectronicfields due to their excellent mechanicalflexibility,low cost,and solution processing.However,grain boundaries(GBs)disrupt the aggrega-tion state of organic semiconductor(OSC)films and hinder electrical performance and stability,which limits the application of OFETs.Besides,the sensitive nature of GBs is widely used in sensing,but detailed descriptions of the GBs are scarce.This review aims tofill this knowledge gap.The role of GBs and their effect on the per-formance and stability of OFETs are analyzed,followed by a detailed summary of the characterization of GBs.Then,strategies for suppressing the negative effects of GBs and utilizing the sensitive nature of GBs for application are proposed.Finally,potential research directions for GBs in OFETs are discussed.

Layer by Layer Self-assembly Fiber-based Flexible Electrochemical Transistor

Poly(3,4-ethylenedioxyethiophene)-polystyrene sulfonic acid(PEDOT:PSS)/polyallyl dimethyl ammonium chloride modified reduced graphene oxide(PDDA-rGO)was layer by layer self-assembled on the cotton fiber.The surface morphology and electric property was investigated.The results confirmed the dense membrane of PEDOT:PSS and the lamellar structure of PDDA-rGO on the fibers.It has excellent electrical conductivity and mechanical properties.The fiber based electrochemical transistor(FECTs)prepared by the composite conductive fiber has a maximum output current of 8.7 mA,a transconductance peak of 10 mS,an on time of 1.37 s,an off time of 1.6 s and excellent switching stability.Most importantly,the devices by layer by layer self-assembly technology opens a path for the true integration of organic electronics with traditional textile technologies and materials,laying the foundation for their later widespread application.

Tactile and temperature sensors based on organic transistors:Towards e-skin fabrication

Tactile and temperature sensors are the key components for e-skin fabrication.Organic transistors,a kind of intrinsic logic devices with diverse internal configurations,offer a wide range of options for sensor design and have played a vital role in the fabrication of e-skin-oriented tactile and temperature sensors.This research field has attained tremendous advancements,both in terms of materials design and device architecture,thereby leading to excellent performance of resulting tactile/temperature sensors.Herein,a systematic review of organic transistor-based tactile and temperature sensors is presented to summarize the latest progress in these devices.Particularly,we focus on spotlighting various device structures,underlying mechanisms and their performance.Lastly,an outlook for the future development of these devices is briefly discussed.We anticipate that this review will provide a quick overview of such a rapidly emerging research direction and attract more dedicated efforts for the development of next-generation sensing devices towards e-skin fabrication.

Fabrication of flexible thin organic transistors by trace water assisted transfer method

The development of fabrication method for flexible thin organic electronic device is highly important for the flexible and wearable products. Herein, we develop a facile peel-off method to transfer organic thin film to various substrates. In this strategy, polyacrylonitrile （PAN） film can be easily peeled offwith trace water and further transferred to various substrates. Using PAN as supporting and dielectric layers, high performance flexible organic transistors are fabricated. Remarkably, the method uses only micro volume water as an assist to peel off PAN film, which reduces the risk of contamination by solvent and greatly contributes to the performance maintenance.

Influence of Temperature and Pentacene Thickness on the Electrical Parameters in Top Gate Organic Thin Film Transistor

In this contribution, we report on the effect of pentacene thickness and temperature on the performance of top gate transistors. We first investigated the temperature dependence of the transport properties in the temperature range of 258 K - 353 K. The electrical characteristics showed that the threshold voltage (VT) and the onset voltage (Von) remain unchanged. However, the subthreshold current (Ioff), the on-current (Ion) and the field effect mobility (μ) are highly affected with a slight deterioration of subthreshold slope. We observed Arrhenius-like behavior suggesting a thermally activated mobility with an activation energy EA = 68 meV. Moreover the dependence of the charge carrier mobility on the organic semiconductor thickness has also been studied. The mobility decreased as the pentacene thickness increases whereas the threshold voltage and Ioff current remain minimally affected. In order to understand the transport properties and in view to put in light morphology peculiarities of pentacene, AFM images were performed. It turns out that the pentacene grain sizes are smaller and disorganized as the film thickness increases, and charge carriers are more prone to be trapped, leading to decrease the field effect mobility and the Ion current. The devices were also tested under bias stress and the transistors with low thicknesses exhibited a relatively good electrical stability compared to those with high pentacene thicknesses. This work points out the influence of temperature, semiconductor thickness and bias stress effect on the device performance and stability of transistor using top gate configuration.

Air-stable ambipolar organic field effect transistors with heterojunction of pentacene and N,N'-bis(4-trifluoromethylben-zyl) perylene-3,4,9,10-tetracarboxylic diimide

Fabrication of ambipolar organic field-effect transistors （OFETs） is essential for the achievement of an organic complementary logic circuit. Ambipolar transports in OFETs with heterojunction structures are realized.We select pentacene as a P-type material and N,N＇-bis（4-trifluoromethylben-zyl）perylene-3,4,9,10-tetracarboxylic diimide （PTCDI-TFB） as a n-type material in the active layer of the OFETs.The field-effect transistor shows highly air-stable ambipolar characteristics with a field-effect hole mobility of 0.18 cm^2/（V·s） and field-effect electron mobility of 0.031 cm^2/（V·s）.Furthermore the mobility only slightly decreases after being exposed to air and remains stable even for exposure to air for more than 60 days.The high electron affinity of PTCDI-TFB and the octadecyltrichlorosilane （OTS） self-assembly monolayer between the SiO2 gate dielectric and the organic active layer result in the observed air-stable characteristics of OFETs with high mobility.The results demonstrate that using the OTS as a modified gate insulator layer and using high electron affinity semiconductor materials are two effective methods to fabricate OFETs with air-stable characteristics and high mobility.

Organic Electrochemical Transistor based on Polypyrrole/ Crosslinked Chitosan/Nylon Fibers

Glutaraldehyde(GA)crosslinked chitosan(CHIT)was modified on nylon fibers.Afterwards,pyrrole was in-situ polymerized on the surface of the CHIT/Nylon fiber.The SEM and FT-IR results show that the functional fiber is successfully prepared,and the obtained polypyrrole(PPy)presents nanorods morphology on the fiber surface.The mechanical properties of the fibers were studied by Instron.The organic electrochemical transistors based on PPy/Nylon fiber,PPy/CHIT/Nylon fiber,and PPy/GA-CHIT/Nylon fiber as channels were prepared and their transistors performance was compared.It is found that PPy/GA-CHIT/Nylon fiber-based transistor has great output,transfer,transient curves,and excellent transconductance of 6.8 mS,providing a new platform for the field of wearable devices.Furthermore,the study introduces chitosan material with excellent biocompatibility,which makes prepared transistors also have potential applications in the field of biosensing.

High performance pentacene organic field-effect transistors consisting of biocompatible PMMA/silk fibroin bilayer dielectric

Pentacene organic field-effect transistors （OFETs） based on single- or double-layer biocompatible dielectrics of poly（methyl methacrylate） （PMMA） and/or silk fibroin （SF） are fabricated. Compared with those devices based on sin- gle PMMA or SF dielectric or SF/PMMA bilayer dielectric, the OFETs with biocompatible PMMA/SF bilayer dielectric exhibit optimal performance with a high field-effect mobility of 0.21 cm2/Vs and a current on/off ratio of 1.5 × 104. By investigating the surface morphology of the pentacene active layer through atom force microscopy and analyzing the elec- trical properties, the performance enhancement is mainly attributed to the crystallization improvement of the pentacene and the smaller interface trap density at the dielectric/organic interface. Meanwhile, a low contact resistance also indicates that a good electrode/organic contact is formed, thereby assisting the performance improvement of the OFET.

Enhanced charge carrier injection in heterojunction organic field-effect transistor by inserting an MoO_3 buffer layer

A top-contact organic field-effect transistor （OFET） is fabricated by adopting a pentacene/1,11-bis（di-4- tolylaminophenyl） cyclohexane （TAPC） heterojunction structure and inserting an MoO3 buffer layer between the TAPC organic semiconductor layer and the source/drain electrode. The performances of the heterojunction OFET, including output current, field-effect mobility, and threshed voltage~ are all significantly improved by introducing the MoO3 thin buffer layer. The performance improvement of the modified heterojunction OFET is attributed to a better contact formed at the Au/TAPC interface due to the MoO3 thin buffer layer, thereby leading to a remarkable reduction of the contact resistance at the metal/organic interface.

Controlled Growth of Large-Area Aligned Single-Crystalline Organic Nanoribbon Arrays for Transistors and Light-Emitting Diodes Driving

Organic field-effect transistors(OFETs) based on organic micro-/nanocrystals have been widely reported with charge carrier mobility exceeding 1.0 cm^2V^(-1)s^(-1), demonstrating great potential for high-performance, low-cost organic electronic applications. However, fabrication of large-area organic micro-/nanocrystal arrays with consistent crystal growth direction has posed a significant technical challenge. Here, we describe a solution-processed dip-coating technique to grow large-area, aligned 9,10-bis(phenylethynyl) anthracene(BPEA) and 6,13-bis(triisopropylsilylethynyl) pentacene(TIPSPEN) single-crystalline nanoribbon arrays. The method is scalable to a 5 9 10 cm^2 wafer substrate, with around 60% of the wafer surface covered by aligned crystals. The quality of crystals can be easily controlled by tuning the dip-coating speed. Furthermore, OFETs based on well-aligned BPEA and TIPS-PEN single-crystalline nanoribbons were constructed.By optimizing channel lengths and using appropriate metallic electrodes, the BPEA and TIPS-PEN-based OFETs showed hole mobility exceeding 2.0 cm^2V^(-1)s^(-1)(average mobility 1.2 cm^2V^(-1)s^(-1)) and 3.0 cm^2V^(-1)s^(-1)(average mobility2.0 cm^2V^(-1)s^(-1)), respectively. They both have a high on/off ratio(I_(on)/I_(off))>10~9. The performance can well satisfy the requirements for light-emitting diodes driving.

n-Channel Organic Transistors Processed from Halogen-Free Solvents： Solvent Effect on Thin-Film Morphology and Charge Transport

Non-chlorinated solvents are highly preferable for organic electronic processing due to their environmentally friendly characteristics. Four different halogen-free solvents, tetrafuran, toluene, meta-xylene and 1,2,4-trimethyl- benzene, were selected to fabricate n-channel organic thin film transistors （OTFTs） based on 3-hexylundecyl sub- stituted naphthalene diimides fused with （1,3-dithiol-2-ylidene）malononitrile groups （NDI3HU-DTYM2）. The OTFTs based on NDI3HU-DTYM2 showed electron mobility of up to 1.37 cm2-V-1·s -1 under ambient condition. This is among the highest device performance for n-channel OTFTs processed from halogen-free solvents. The dif- ferent thin-film morphologies, from featureless low crystalline morphology to well-aligned nanofibres, have a great effect on the device performance. These results might shed some light on solvent selection and the resulting solution process for organic electronic devices.

Thickness dependence of surface morphology and charge carrier mobility in organic field-effect transistors

With the aim of understanding the relationships between organic small molecule field-effect transistors （FETs） and organic conjugated polymer FETs, we investigate the thickness dependence of surface morphology and charge carrier mobility in pentacene and regioregular poly （3-hexylthiophene） （RR-P3HT） field-effect transistors. On the basis of the results of surface morphologies and electrical properties, we presume that the charge carrier mobility is largely related to the morphology of the organic active layer. We observe that the change trends of the surface morphologies （average size and average roughness） of pentacene and RR-P3HT thin films are mutually opposite, as the thickness of the organic layer increases. Further, we demonstrate that the change trends of the field-effect mobilities of pentacene and RR-P3HT FETs are also opposite to each other, as the thickness of the organic layer increases within its limit.

Study of top and bottom contact resistance in one organic field-effect transistor

This paper reports that the organic field-effect transistors with hybrid contact geometry were fabricated, in which the top electrodes and the bottom electrodes were combined in parallel resistances within one transistor. With the facility of the novel structure, the difference of contact resistance between the top contact geometry and the bottom contact geometry was studied. The hybrid contact devices showed similar characteristics with the top contact configuration devices, which provide helpful evidence on the lower contact resistance of the top contact configuration device. The origin of the different contact resistance between the top contact device and the bottom contact device was discussed.

Study on characteristics of a double-conductible channel organic thin-film transistor with an ultra-thin hole-blocking layer

The properties of top-contact organic thin-film transistors （TC-OTFTs） using ultra-thin 2, 9-dimethyl-4, 7- diphenyl-1, 10-phenanthroline （BCP） as a hole-blocking interlayer have been improved significantly and a BCP interlayer was inserted into the middle of the pentacene active layer. This paper obtains a fire-new transport mode of an OTFT device with double-conductible channels. The accumulation and transfer of the hole carriers arc limited by the BCP interlayer in the vertical region of the channel. A huge amount of carriers is located not only at the interface between pentacene and the gate insulator, but also at the two interfaces of pentacene/BCP interlayer and pentacene/gate insulator, respectively. The results suggest that the BCP interlayer may be useful to adjust the hole accumulation and transfer, and can increase the hole mobility and output current of OTFTs. The TC-OTFTs with a BCP interlayer at VDS = --20 V showed excellent hole mobility μFE and threshold voltage VTH of 0.58 cm^2/（V-s） and -4.6 V, respectively.

Application of graphene vertical field effect to regulation of organic light-emitting transistors

The luminescence intensity regulation of organic light-emitting transistor(OLED)device can be achieved effectively by the combination of graphene vertical field effect transistor(GVFET)and OLED.In this paper,we fabricate and characterize the graphene vertical field-effect transistor with gate dielectric of ion-gel film,confirming that its current switching ratio reaches up to 102.Because of the property of high light transmittance in ion-gel film,the OLED device prepared with graphene/PEDOT:PSS as composite anode exhibits good optical properties.We also prepare the graphene vertical organic light-emitting field effect transistor(GVOLEFET)by the combination of GVFET and graphene OLED,analyzing its electrical and optical properties,and confirming that the luminescence intensity can be significantly changed by regulating the gate voltage.

Top contact organic field effect transistors fabricated using a photolithographic process

This paper proposes an effective method of fabricating top contact organic field effect transistors by using a pho- tolithographic process. The semiconductor layer is protected by a passivation layer. Through photolithographic and etching processes, parts of the passivation layer are etched off to form source/drain electrode patterns. Combined with conventional evaporation and lift-off techniques, organic field effect transistors with a top contact are fabricated suc- cessfully, whose properties are comparable to those prepared with the shadow mask method and one order of magnitude higher than the bottom contact devices fabricated by using a photolithographic process.

Performance improvement in pentacene organic thin film transistors by inserting a C_(60) ultrathin layer

The contact effect on the performances of organic thin film transistors is studied here. A C60 ultrathin layer is inserted between Al source-drain electrode and pentacene to reduce the contact resistance. By a 3 nm C60 modification, the injection barrier is lowered and the contact resistance is reduced. Thus, the field-effect mobility increases from 0.12 to 0.52 cm2/（V.s）. It means that inserting a C60 ultra thin layer is a good method to improve the organic thin film transistor （OTFT） performance. The output curve is simulated by using a charge drift model. Considering the contact effect, the field effect mobility is improved to 1.15 cm2/（V-s）. It indicates that further reducing the contact resistance of OTFTs should be carried out.