Improved Performance in Diketopyrrolopyrrole-Based Transistors with Bilayer Gate Dielectrics

There has been significant progress in the past 2 decades in the field of organic and polymer thin-film transistors. In this paper, we report a combination of stable materials, device architecture, and process conditions that resulted in a patterned gate, small channel length (<5 μm) device that possesses a scaled field-induced conductivity in air that is higher than any organic/polymer transistor reported thus far. The operating voltage is below 10 V; the on-off ratio is high; and the active materials are solution-processable. The semiconducting polymer is a new donor–acceptor polymer with furan-substituted diketopyrrolopyrrole and thienyl-vinylene-thienyl building blocks in the conjugated backbone. One of the major striking features of our work is that the patterned-gate device architecture is suitable for practical applications. We also propose a figure of merit to meaningfully compare polymer/organic transistor performance that takes into account mobility and operating voltage. With this figure of merit, we compare leading organic and polymer transistors that have been hitherto reported. The material and device architecture have shown very high mobility and low operating voltage for such short channel length (below 5 μm) organic/polymer transistors

Chemical Understanding of the Mechanisms Involved in Mitigation of Charged Impurity Effects by Polar Molecules on Graphene

It is well-known that the transport properties of monolayer graphene are degraded by charged impurities present between graphene and either a given substrate or air. Such impurities cause charge scattering of holes and electrons in graphene. In previous work, our group has used both fluoropolymer thin films and polar vapor molecules to dramatically improve graphene field-effect transistor (FET) device characteristics, including Dirac voltage and mobility. We attributed the graphene device improvements to mitigation of charged impurities and defects due to electrostatic interaction with the dipoles of the applied fluoropolymers and polar molecules. In this work, we present theoretical support to this hypothesis, in the form of computational chemical simulations involving the interaction of polar molecules and impurities on a graphene sheet. We examine two types of impurities which may occur at graphene interfaces: ionic impurities and molecular dipole impurities. Upon introduction of polar vapor molecules to an impurity/graphene system, we observed a dramatic reduction in the electrostatic potential in the plane of the graphene from the impurity. The magnitude of potential reduction scales with the average dipole moment of each polar molecule. We were able to determine two separate mechanisms which contribute to the total potential reduction, impurity displacement, and electrostatic screening of the impurity. The respective impacts of the mechanisms vary with distance from the impurity. Additionally, in the case of the molecular dipole impurity, the orientation of the impurity atop graphene is a key factor that determines the potential impact

High-Speed, Inkjet-Printed Carbon Nanotube/Zinc Tin Oxide Hybrid Complementary Ring Oscillators

The materials combination of inkjet-printed single-walled carbon nanotubes (SWCNTs) and zinc tin oxide (ZTO) is very promising for large-area thin-film electronics. We compare the characteristics of conventional complementary inverters and ring oscillators measured in air (with SWCNT p-channel field effect transistors (FETs) and ZTO n-channel FETs) with those of ambipolar inverters and ring oscillators comprised of bilayer SWCNT/ZTO FETs. This is the first such comparison between the performance characteristics of ambipolar and conventional inverters and ring oscillators. The measured signal delay per stage of 140 ns for complementary ring oscillators is the fastest for any ring oscillator circuit with printed semiconductors to date

Transformation of the Electrical Characteristics of Graphene Field-Effect Transistors with Fluoropolymer

We report on the improvement of the electronic characteristics of monolayer graphene field-effect transistors (FETs) by an interacting capping layer of a suitable fluoropolymer. Capping of monolayer graphene FETs with CYTOP improved the on–off current ratio from 5 to 10 as well as increased the field-effect mobility by as much as a factor of 2 compared to plain graphene FETs. Favorable shifts in the Dirac voltage toward zero with shift magnitudes in excess of 60 V are observed. The residual carrier concentration is reduced to ∼2.8 × 10¹¹ cm^–2. Removal of the fluoropolymer from graphene FETs results in a return to the initial electronic properties before depositing CYTOP. This suggests that weak, reversible electronic perturbation of graphene by the fluoropolymer favorably tune the electrical characteristics of graphene, and we hypothesize that the origin of this improvement is in the strongly polar nature of the C–F chemical bonds that self-organize upon heat treatment. We demonstrate a general method to favorably restore or transform the electrical characteristics of graphene FETs, which will open up new applications

Efficient Polymer Solar Cells Enabled by Low Temperature Processed Ternary Metal Oxide as Electron Transport Interlayer with Large Stoichiometry Window

Highly efficient organic photovoltaic cells are demonstrated by incorporating low temperature solution processed indium zinc oxide (IZO) as cathode interlayers. The IZOs are synthesized using a combustion synthesis method, which enables low temperature processes (150–250 °C). We investigated the IZO films with different electron mobilities (1.4 × 10^–3 to 0.23 cm²/(V·s)), hydroxide–oxide content (38% to 47%), and surface roughness (0.19–5.16 nm) by modulating the ternary metal oxide stoichiometry. The photovoltaic performance was found to be relatively insensitive to the composition ratio of In:Zn over the range of 0.8:0.2 to 0.5:0.5 despite the differences in their electrical and surface properties, achieving high power conversion efficiencies of 6.61%–7.04%. Changes in composition ratio of IZO do not lead to obvious differences in energy levels, diode parameters and morphology of the photoactive layer, as revealed by ultraviolet photoelectron spectroscopy (UPS), dark current analysis and time-of-flight secondary ion mass spectrometry (TOF-SIMS) measurements, correlating well with the large IZO stoichiometry window that enables efficient photovoltaic devices. Our results demonstrate the robustness of this ETL system and provide a convenient approach to realize a wide range of multicomponent oxides and compatible with processing on flexible plastic substrates

Enhanced Photoresponse in Metasurface-Integrated Organic Photodetectors

In this work, we experimentally demonstrate metasurface-enhanced photoresponse in organic photodetectors. We have designed and integrated a metasurface with broadband functionality into an organic photodetector, with the goal of significantly increasing the absorption of light and generated photocurrent from 560 up to 690 nm. We discuss how the metasurface can be integrated with the fabrication of an organic photodiode. Our results show large gains in responsivity from 1.5× to 2× between 560 and 690 nm

25 GHz Embedded-Gate Graphene Transistors with High‑K Dielectrics on Extremely Flexible Plastic Sheets

Despite the widespread interest in graphene electronics over the past decade, high-performance graphene field-effect transistors (GFETs) on flexible substrates have been rarely achieved, even though this atomic sheet is widely understood to have greater prospects for flexible electronic systems. In this article, we report detailed studies on the electrical and mechanical properties of vapor synthesized high-quality monolayer graphene integrated onto flexible polyimide substrates. Flexible graphene transistors with high-k dielectric afforded intrinsic gain, maximum carrier mobilities of 3900 cm²/V·s, and importantly, 25 GHz cutoff frequency, which is more than a factor of 2.5 times higher than prior results. Mechanical studies reveal robust transistor performance under repeated bending, down to 0.7 mm bending radius, whose tensile strain is a factor of 2–5 times higher than in prior studies. In addition, integration of functional coatings such as highly hydrophobic fluoropolymers combined with the self-passivation properties of the polyimide substrate provides water-resistant protection without compromising flexibility, which is an important advancement for the realization of future robust flexible systems based on graphene

Long-Term Stability and Reliability of Black Phosphorus Field-Effect Transistors

Black phosphorus has been recently suggested as a very promising material for use in 2D field-effect transistors. However, due to its poor stability under ambient conditions, this material has not yet received as much attention as for instance MoS₂. We show that the recently demonstrated Al₂O₃ encapsulation leads to highly stable devices. In particular, we report our long-term study on highly stable black phosphorus field-effect transistors, which show stable device characteristics for at least eight months. This high stability allows us to perform a detailed analysis of their reliability with respect to hysteresis as well as the arguably most important reliability issue in silicon technologies, the bias-temperature instability. We find that the hysteresis in these transistors depends strongly on the sweep rate and temperature. Moreover, the hysteresis dynamics in our devices are reproducible over a long time, which underlines their high reliability. Also, by using detailed physical models for oxide traps developed for Si technologies, we are able to capture the channel electrostatics of the black phosphorus FETs and determine the position of the defect energy band. Finally, we demonstrate that both hysteresis and bias-temperature instabilities are due to thermally activated charge trapping/detrapping by oxide traps and can be reduced if the device is covered by Teflon-AF

25 GHz Embedded-Gate Graphene Transistors with High‑K Dielectrics on Extremely Flexible Plastic Sheets

Despite the widespread interest in graphene electronics over the past decade, high-performance graphene field-effect transistors (GFETs) on flexible substrates have been rarely achieved, even though this atomic sheet is widely understood to have greater prospects for flexible electronic systems. In this article, we report detailed studies on the electrical and mechanical properties of vapor synthesized high-quality monolayer graphene integrated onto flexible polyimide substrates. Flexible graphene transistors with high-k dielectric afforded intrinsic gain, maximum carrier mobilities of 3900 cm²/V·s, and importantly, 25 GHz cutoff frequency, which is more than a factor of 2.5 times higher than prior results. Mechanical studies reveal robust transistor performance under repeated bending, down to 0.7 mm bending radius, whose tensile strain is a factor of 2–5 times higher than in prior studies. In addition, integration of functional coatings such as highly hydrophobic fluoropolymers combined with the self-passivation properties of the polyimide substrate provides water-resistant protection without compromising flexibility, which is an important advancement for the realization of future robust flexible systems based on graphene

Logic-Gate Devices Based on Printed Polymer Semiconducting Nanostripes

The applications of organic semiconductors in complex circuitry such as printed CMOS-like logic circuits demand miniaturization of the active structures to the submicrometric and nanoscale level while enhancing or at least preserving the charge transport properties upon processing. Here, we addressed this issue by using a wet lithographic technique, which exploits and enhances the molecular order in polymers by spatial confinement, to fabricate ambipolar organic field effect transistors and inverter circuits based on nanostructured single component ambipolar polymeric semiconductor. In our devices, the current flows through a precisely defined array of nanostripes made of a highly ordered diketopyrrolopyrrole-benzothiadiazole copolymer with high charge carrier mobility (1.45 cm² V^–1 s^–1 for electrons and 0.70 cm² V^–1 s^–1 for holes). Finally, we demonstrated the functionality of the ambipolar nanostripe transistors by assembling them into an inverter circuit that exhibits a gain (105) comparable to inverters based on single crystal semiconductors