Enabling gate dielectric design for all solution-processed, high-performance, flexible organic thin-film transistors

A novel solution-processed, compositionally and structurally stable dual-layer gate dielectric composed of a UV-cured poly(4-vinyl phenol)-co-poly(methyl methacrylate) bottom layer and a thermally cross-linked poly(methyl silsesquioxane) top layer for organic thin-film transistors is described. This gate dielectric design, coupled with compatible solution-processable semiconductor and conductor materials, has enabled fabrication of all solution-processed, high-performance organic thin-film transistors on flexible substrates. High field-effect mobility and current on/off ratio, together with other desirable transistor properties, are demonstrated.     

Theoretical study of the source-drain current and gate leakage current to understand the graphene field-effect transistors

We designed acene molecules attached to two semi-infinite metallic electrodes to explore the source-drain current of graphene and the gate leakage current of the gate dielectric material in the field-effect transistors (FETs) device using the first-principles density functional theory combined with the non-equilibrium Green's function formalism. In the acene-based molecular junctions, we modify the connection position of the thiol group at one side, forming different electron transport routes. The electron transport routes besides the shortest one are defined as the cross channels. The simulation results indicate that electron transport through the cross channels is as efficient as that through the shortest one, since the conductance is weakly dependent on the distance. Thus, it is possible to connect the graphene with multiple leads, leading the graphene as a channel utilized in the graphene-based FETs in the mesoscopic system. When the conjugation of the cross channel is blocked, the junction conductance decreases dramatically. The differential conductance of the BA-1 is nearly 7 (54.57 μS) times as large as that of the BA-4 (7.35 μS) at zero bias. Therefore, the blocked graphene can be employed as the gate dielectric material in the top-gated graphene FET device, since the leakage current is small. The graphene-based field-effect transistors fabricated with a single layer of graphene as the channel and the blocked graphene as the gate dielectric material represent one way to overcome the problem of miniaturization which faces the new generation of transistors.     

High-performance organic field-effect transistors: molecular design, device fabrication, and physical properties

In the past decade, tremendous progress has been made in organic field-effect transistors (OFETs). Their real applications require further development of device performance. OFETs consist of organic semiconductors, dielectric layers, and electrodes. Organic semiconductors play a key role in determining the device characteristics. The properties of the organic semiconductors, such as molecular structure and packing, as well as molecular energy levels, can be properly controlled by molecular design. Therefore, we designed and synthesized a series of organic molecules. The synthesized organic semiconductors exhibit excellent field-effect properties due to strong intermolecular interactions and proper molecular energy levels. Meanwhile, the influence of the device fabrication process, organic semiconductor/dielectric layer interface, and organic layer/electrode contact on the device performance was investigated. A deep understanding of these factors is helpful to improve field-effect properties. Furthermore, single-crystal field-effect transistors are highlighted because the single-crystal-based FETs can provide an accurate conducting mechanism of organic semiconductors and higher device performance as compared with thin film FETs.     

Air-assisted high-performance field-effect transistor with thin films of picene

A field-effect transistor (FET) with thin films of picene has been fabricated on SiO2 gate dielectric. The FET showed p-channel enhancement-type FET characteristics with the field-effect mobility, mu, of 1.1 cm2 V-1 s-1 and the on-off ratio of >10(5). This excellent device performance was realized under atmospheric conditions. The mu increased with an increase in temperature, and the FET performance was improved by exposure to air or O2 for a long time. This result implies that this device is an air (O2)-assisted FET. The FET characteristics are discussed on the basis of structural topography and the energy diagram of picene thin films.     

Toward quantifying the electrostatic transduction mechanism in carbon nanotube molecular sensors

Despite the great promise of carbon nanotube field-effect transistors (CNT FETs) for applications in chemical and biochemical detection, a quantitative understanding of sensor responses is lacking. To explore the role of electrostatics in sensor transduction, experiments were conducted with a set of highly similar compounds designed to adsorb onto the CNT FET via a pyrene linker group and take on a set of known charge states under ambient conditions. Acidic and basic species were observed to induce threshold voltage shifts of opposite sign, consistent with gating of the CNT FET by local charges due to protonation or deprotonation of the pyrene compounds by interfacial water. The magnitude of the gate voltage shift was controlled by the distance between the charged group and the CNT. Additionally, functionalization with an uncharged pyrene compound showed a threshold shift ascribed to its molecular dipole moment. This work illustrates a method for producing CNT FETs with controlled values of the turnoff gate voltage, and more generally, these results will inform the development of quantitative models for the response of CNT FET chemical and biochemical sensors.     

基于CH3NH3PbI3单晶的Ta2O5顶栅双极性场效应晶体管

Organic-inorganic hybrid perovskite methylammonium lead iodide (CH₃NH₃PbI₃) generally tends to show n-type semiconductor properties. In this work, a field-effect transistor (FET) device based on a CH₃NH₃PbI₃ single crystal with tantalum pentoxide (Ta₂O₅) as the top gate dielectric was fabricated. The p-type field-effect transport properties of the device were observed in the dark. The hole mobility of the device extracted from transfer characteristics in the dark was 8.7×10^-5 cm²·V^-1·s^-1, which is one order of magnitude higher than that of polycrystalline FETs with SiO₂ as the bottom gate dielectric. In addition, the effect of light illumination on the CH₃NH₃PbI₃ single-crystal FET was studied. Light illumination strongly influenced the field effect of the device because of the intense photoelectric response of the CH₃NH₃PbI₃ single crystal. Different from a CH₃NH₃PbI₃ polycrystalline FET with a bottom gate dielectric, even with the top gate dielectric shielding, light illumination of 5.00 mW·cm^-2 caused the hole current to increase by one order of magnitude compared with that in the dark (V_GS (gate-source voltage)=V_DS (drain-source voltage)=20 V) and the photoresponsivity reached 2.5 A·W^-1. The introduction of Ta₂O₅ as the top gate dielectric selectively enhanced hole transport in the single-crystal FET, indicating that in the absence of external factors, by appropriate device design, CH₃NH₃PbI₃ also has potential for use in ambipolar transistors.     

ISFETs with sputtered sodium alumino-silicate glass membranes

Sodium ion sensitive field-effect transistors (ISFETs) based on reactively sputtered sodium aluminosilicate (NAS) glass membranes are investigated. Using an inverted cylindrical magnetron, NAS films with defined and reproducible composition are obtained. Radiation damage in the gate dielectric is largely eliminated by annealing at 450 degrees C. The Na(+) sensitivity, the selectivity with respect to H(+) and K(+) ions, the response time, the conditioning period, the long-term drift, and the lifetime are evaluated. The ISFETs exhibit a near-Nernstian Na(+) response down to 10(-4) mol/l in solutions of pH>/=7. The NAS films are physically very robust and have excellent chemical durability, e.g., a sensor with a 110 nm thick membrane lasts for about 8 months. The overall sensor properties compare well with those of a commercial Na(+) selective glass electrode.     

Polymer electrolyte-gated organic field-effect transistors: low-voltage, high-current switches for organic electronics and testbeds for probing electrical transport at high charge carrier density

We report the fabrication and extensive characterization of solid polymer electrolyte-gated organic field-effect transistors (PEG-FETs) in which a polyethylene oxide (PEO) film containing a dissolved Li salt is used to modulate the hole conductivity of a polymer semiconductor. The large capacitance (approximately 10 microF/cm2) of the solution-processed polymer electrolyte gate dielectric facilitates polymer semiconductor conductivities on the order of 103 S/cm at low gate voltages (<3 V). In PEG-FETs based on regioregular poly(3-hexylthiophene), gate-induced hole densities were 2 x 10(14) charges/cm2 with mobilities >3 cm2/V.s. PEG-FETs fabricated with gate electrodes either aligned or intentionally nonaligned to the channel exhibited dramatically different electrical behavior when tested in vacuum or in air. Large differences in ionic diffusivity can explain the dominance of either electrostatic charging (in vacuum) or bulk electrochemical doping (in air) as the device operational mechanism. The use of a larger anion in the polymer electrolyte, bis(trifluoromethanesulfonyl)imide (TFSI-), yielded transistors that showed clear current saturation and square law behavior in the output characteristics, which also points to electrostatic (field-effect) charging. In addition, negative transconductances were observed using the PEO/LiTFSI electrolyte for all three polymer semiconductors at gate voltages larger than -3 V. Bias stress measurements performed with PEO/LiTFSI-gated bottom contact PEG-FETs showed that polymer semiconductors can sustain high ON currents for greater than 10 min without large losses in conductance. Collectively, the results indicate that PEG-FETs may serve as useful devices for high-current/low-voltage applications and as testbeds for probing electrical transport in polymer semiconductors at high charge density.     

Vapor phase self-assembly of molecular gate dielectrics for thin film transistors

Organic-inorganic films grown entirely via a vapor-phase deposition process and composed of highly polarizable molecular structures are investigated as gate dielectrics in organic field-effect transistors (OFETs). Molecules 1 and 2 form self-ordered thin films via hydrogen bonding, and these organic-inorganic structures exhibit large capacitances and large pentacene OFET mobilities.     

High-mobility graphene nanoribbons prepared using polystyrene dip-pen nanolithography

Graphene nanoribbons (GNRs) are fabricated by dip-pen nanolithography and polystyrene etching techniques on a SrTiO(3)/Nb-doped SrTiO(3) substrate. A GNR field-effect transistor (FET) shows bipolar FET behavior with a high mobility and low operation voltage at room temperature because of the atomically flat surface and the large dielectric constant of the insulating SrTiO(3) layer, respectively.     

Charge carrier transport in high purity perylene single crystal studied by time-of-flight measurements and through field effect transistor characteristics

Electronic transport has been studied by measuring the characteristics of field effect transistors using high purity perylene and the results have been compared with those from time-of-flight measurements. The purity of the material has been monitored by carrier trapping time and delayed fluorescence lifetime. Three types of field effect transistors have been studied: (1) thin film transistor, (2) transistor prepared by placing a single crystal flake on a substrate and (3) transistor fabricated on a single crystal by depositing electrodes and insulating layer onto it. Compared to thin film transistors prepared by evaporating perylene onto a SiO₂/Si substrate, higher mobility values were obtained with transistors using single crystals, but the electrical characteristics of the transistors were far from ideal: large threshold gate voltage observed in the second class of FETs indicated that a high density of traps are present at the interface between the organics and the insulator. A transistor of the third class showed that it functioned indeed as a FET with a reasonably high mobility, but the operation was not stable enough to allow reliable measurements. Much remains to be improved in the design and construction of a perylene FET before the potentiality of the material is fully developed. Also, it remains to be explored to what extent the bulk purity and the molecular order at the organics/insulator interface influence the transport of the charge carriers in an organic FET.     

硅基超薄多孔氧化铝膜的制备

将二次阳极氧化法应用于硅基铝膜的制备, 在草酸溶液中得到了厚度可控的硅基超薄多孔氧化铝膜(PAM), 厚度小于100 nm. 实验中记录了氧化电流随时间的实时变化曲线, 发现硅衬底的氧化电流在大幅下降前有一小幅波动. 对应于Al/Si界面的氧化过程中, 孔洞底部之间的残留铝岛被优先氧化, 可将此作为终止铝氧化的标志. 扫描电镜(SEM)观察表明, 二次氧化提高了孔洞分布的均匀性, 使得孔在一定的区域内呈现有序六角分布.这种模板可进一步用于硅基纳米器件和纳米结构的制备.     

Photoresponsive organic field-effect transistors involving photochromic molecules

In recent years, organic field-effect transistors (OFETs) with high performance and novel multifunctionalities have attracted considerable attention. Meanwhile, featured with reversible photoisomerization and the corresponding variation in color, chemical/physical properties, photochromic molecules have been applied in sensors, photo-switches and memories. Incorporation of photochromic molecules to blend in the device functional layers or to modify the interfaces of OFETs is common way to build photo-transistors. In this review, we focus on the recent advantages on the study of photoresponsive transistors involving one of three typical photochromic compounds spiropyran, diarylethene and azobenzene. Three main strategies are demonstrated in detail. Firstly, photochromic molecules are doped in active layers or combined with semiconductor structure thus forming photoreversible active layers. Secondly, the modification of dielectric layer/active layer interface is mainly carried out by bilayer dielectric. Thirdly, the photo-isomerization of self-assembled monolayer (SAM) on the electrode/active layer interface can reversibly modulate the work functions and charge injection barrier, result in bifunctional OFETs. All in all, the combination of photochromic molecules and OFETs is an efficient way for the fabrication of organic photoelectric devices. Photoresponsive transistors consisted of photochromic molecules are potential candidate for real applications in the future.     

2,5-二(2-菲基)-[3,2-b]并二噻吩的合成、表征及在有机薄膜晶体管中的应用

本文合成了2,5-二(2-菲基)-[3,2-b]并二噻吩(PhTT), 表征了其基本的物理和化学性质, 制备了相应的有机薄膜晶体管.     

Effect of morphology on organic thin film transistor sensors

This review provides a general introduction to organic field-effect transistors and their application as chemical sensors. Thin film transistor device performance is greatly affected by the molecular structure and morphology of the organic semiconductor layer. Various methods for organic semiconductor deposition are surveyed. Recent progress in the fabrication of organic thin film transistor sensors as well as the correlation between morphology and analyte response is discussed.     

AFM,ellipsometry, XPS and TEM on ultra-thin oxide/polymer nanocomposite layers in organic thin film transistors

Here we report on the fabrication and characterization of ultra-thin nanocomposite layers used as gate dielectric in low-voltage and high-performance flexible organic thin film transistors (oTFTs). Reactive sputtered zirconia layers were deposited with low thermal exposure of the substrate and the resulting porous oxide films with high leakage currents were spin-coated with an additional layer of poly-α-methylstyrene (PαMS). After this treatment a strong improvement of the oTFT performance could be observed; leakage currents could be eliminated almost completely. In ellipsometric studies a higher refractive index of the ZrO₂/PαMS layers compared to the “as sputtered” zirconia films could be detected without a significant enhancement of the film thickness. Atomic force microscopy (AFM) measurements of the surface topography clearly showed a surface smoothing after the PαMS coating. Further studies with X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) also indicated that the polymer definitely did not form an extra layer. The polymer chains rather (self-)assemble in the nano-scaled interspaces of the porous oxide film giving an oxide–polymer “nanocomposite” with a high oxide filling grade resulting in high dielectric constants larger than 15. The dielectric strength of more than 1 MV cm⁻¹ is in good accordance with the polymer-filled interspaces.     

Fabrication of organic thin-film transistors using layer-by-layer assembly

Layer-by-layer assembly is presented as a deposition technique for the incorporation of ultrathin gate dielectric layers into thin-film transistors utilizing a highly doped organic active layer. This deposition technique enables the fabrication of device structures with a controllable gate dielectric thickness. In particular, devices with a dielectric layer comprised of poly(allylamine hydrochloride)/poly(acrylic acid) (PAH/PAA) bilayer films were fabricated to examine the properties of poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) as the transistor active layer. The transistor Ion/off ratio and switching speed are shown to be controlled by the gate bias, which is dependent upon the voltage applied and the number of bilayers deposited for the gate dielectric. The devices operate in the depletion mode as a result of dedoping of the active layer with the application of a positive gate bias. The depletion and recovery rate are highly dependent on the level of hydration in the film and the environment under which the device is operated. These observations are consistent with an electrochemical dedoping of the conducting polymer during operation.     

A quantitative analytical model for static dipolar disorder broadening of the density of states at organic heterointerfaces

Understanding the electronic structure of organic-organic heterointerfaces is crucial for many device applications of organic semiconductors. Here we have developed a simple analytical model to describe the effect of static dipolar disorder in a polymer dielectric on the density of states of an adjacent organic semiconductor. The degree of energetic disorder varies strongly with distance from the interface. Using a simple mobility model, we have been able to explain quantitatively both the magnitude as well as the gate voltage dependence of the field-effect mobility for polymer gate dielectrics with different dielectric constants.     

聚合物场效应晶体管材料及其器件

导电聚合物因为可以大面积成膜、器件制作工艺简单,近年来在有机场效应晶体管的研究中受到越来越多的关注。有的聚合物场效应晶体管其性能已经可以和无定型硅晶体管相比拟。本文回顾了聚合物场效应晶体管的发展历程,概述了聚合物场效应晶体管的材料、器件制作、性能及工作机理。同时,对聚合物场效应晶体管的发展前景和目前存在的问题作了简单的总结。     

聚合物场效应晶体管材料及其器件

导电聚合物因为可以大面积成膜、器件制作工艺简单,近年来在有机场效应晶体管的研究中受到越来越多的关注.有的聚合物场效应晶体管其性能已经可以和无定型硅晶体管相比拟.本文回顾了聚合物场效应晶体管的发展历程,概述了聚合物场效应晶体管的材料、器件制作、性能及工作机理.同时,对聚合物场效应晶体管的发展前景和目前存在的问题作了简单的总结.