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Printed systems spark immense interest in industry, and for several parts such as solar cells or radio frequency identification antennas, printed products are already available on the market. This has led to intense research; however, printed field-effect transistors (FETs) and logics derived thereof still have not been sufficiently developed to be adapted by industry. Among others, one of the reasons for this is the lack of control of the threshold voltage during production. In this work, we show an approach to adjust the threshold voltage (Vth) in printed electrolyte-gated FETs (EGFETs) with high accuracy by doping indium-oxide semiconducting channels with chromium. Despite high doping concentrations achieved by a wet chemical process during precursor ink preparation, good on/off-ratios of more than five orders of magnitude could be demonstrated. The synthesis process is simple, inexpensive, and easily scalable and leads to depletion-mode EGFETs, which are fully functional at operation potentials below 2 V and allows us to increase Vth by approximately 0.5 V.
Silicon (Si) has turned out to be a promising active material for next‐generation lithium‐ion battery anodes. Nevertheless, the issues known from Si as electrode material (pulverization effects, volume change etc.) are impeding the development of Si anodes to reach market maturity. In this study, we are investigating a possible application of Si anodes in low‐power printed electronic applications. Tailored Si inks are produced and the impact of carbon coating on the printability and their electrochemical behavior as printed Si anodes is investigated. The printed Si anodes contain active material loadings that are practical for powering printed electronic devices, like electrolyte gated transistors, and are able to show high capacity retentions. A capacity of 1754 mAh/gSi is achieved for a printed Si anode after 100 cycles. Additionally, the direct applicability of the printed Si anodes is shown by successfully powering an ink‐jet printed transistor.
Printed electronics (PE) circuits have several advantages over silicon counterparts for the applications where mechanical flexibility, extremely low-cost, large area, and custom fabrication are required. The custom (personalized) fabrication is a key feature of this technology, enabling customization per application, even in small quantities due to low-cost printing compared with lithography. However, the personalized and on-demand fabrication, the non-standard circuit design, and the limited number of printing layers with larger geometries compared with traditional silicon chip manufacturing open doors for new and unique reverse engineering (RE) schemes for this technology. In this paper, we present a robust RE methodology based on supervised machine learning, starting from image acquisition all the way to netlist extraction. The results show that the proposed RE methodology can reverse engineer the PE circuits with very limited manual effort and is robust against non-standard circuit design, customized layouts, and high variations resulting from the inherent properties of PE manufacturing processes.
Emerging applications in soft robotics, wearables, smart consumer products or IoT-devices benefit from soft materials, flexible substrates in conjunction with electronic functionality. Due to high production costs and conformity restrictions, rigid silicon technologies do not meet application requirements in these new domains. However, whenever signal processing becomes too comprehensive, silicon technology must be used for the high-performance computing unit. At the same time, designing everything in flexible or printed electronics using conventional digital logic is not feasible yet due to the limitations of printed technologies in terms of performance, power and integration density. We propose to rather use the strengths of neuromorphic computing architectures consisting in their homogeneous topologies, few building blocks and analog signal processing to be mapped to an inkjet-printed hardware architecture. It has remained a challenge to demonstrate non-linear elements besides weighted aggregation. We demonstrate in this work printed hardware building blocks such as inverter-based comprehensive weight representation and resistive crossbars as well as printed transistor-based activation functions. In addition, we present a learning algorithm developed to train the proposed printed NCS architecture based on specific requirements and constraints of the technology.
Printed electrolyte-gated oxide electronics is an emerging electronic technology in the low voltage regime (≤1 V). Whereas in the past mainly dielectrics have been used for gating the transistors, many recent approaches employ the advantages of solution processable, solid polymer electrolytes, or ion gels that provide high gate capacitances produced by a Helmholtz double layer, allowing for low-voltage operation. Herein, with special focus on work performed at KIT recent advances in building electronic circuits based on indium oxide, n-type electrolyte-gated field-effect transistors (EGFETs) are reviewed. When integrated into ring oscillator circuits a digital performance ranging from 250 Hz at 1 V up to 1 kHz is achieved. Sequential circuits such as memory cells are also demonstrated. More complex circuits are feasible but remain challenging also because of the high variability of the printed devices. However, the device inherent variability can be even exploited in security circuits such as physically unclonable functions (PUFs), which output a reliable and unique, device specific, digital response signal. As an overall advantage of the technology all the presented circuits can operate at very low supply voltages (0.6 V), which is crucial for low-power printed electronics applications.
Electrolyte-gated thin-film transistors (EGTs) with indium oxide channel, and expected lifetime of three months, enable low-voltage operation (~1 V) in the field of printed electronics (PEs). The channel width of our printed EGTs is varied between 200 and 1000 μm, whereas a channel length between 10 and 100 μm is used. Due to the lack of uniform performance p-type metal oxide semiconductors, n-type EGTs and passive elements are used to design circuits. For logic gates, transistor-resistor logic has been employed so far, but depletion and enhancement-mode EGTs in a transistor-transistor logic boost the circuit performance in terms of delay and signal swing. In this article, the threshold voltage of the EGT, which determines the operation mode, is tuned through sizing of the EGTs channel geometry. The feasibility of both transistor operation modes is demonstrated for logic gates and ring oscillators. An inverter operating at a supply voltage of 1 V shows a maximum gain of 9.6 and a propagation delay time of 0.7 ms, which represents an improvement of ~ 2x for the gain and oscillation frequency, in comparison with the resistor-transistor logic design. Moreover, the power consumption is reduced by 6x.
Printed electronics can benefit from the deployment of electrolytesas gate insulators,which enables a high gate capacitance per unit area (1–10 μFcm−2) due to the formation of electrical double layers (EDLs). Consequently, electrolyte-gated field-effect transistors (EGFETs) attain high-charge carrier densities already in the subvoltage regime, allowing for low-voltage operation of circuits and systems. This article presents a systematic study of lumped terminal capacitances of printed electrolyte-gated transistors under various dc bias conditions. We perform voltage-dependent impedancemeasurements and separate extrinsic components from the lumped terminal capacitance.
The proposed Meyer-like capacitance model, which also accounts for the nonquasi-static (NQS) effect, agrees well with experimental data. Finally, to verify the model, we implement it in Verilog-A and simulate the transient response of an inverter and a ring oscillator circuit. Simulation results are in good agreement with the measurement data of fabricated devices.
Morphological transition of a rod-shaped phase into a string of spherical particles is commonly observed in the microstructures of alloys during solidification (Ratke and Mueller, 2006). This transition phenomenon can be explained by the classic Plateau-Rayleigh theory which was derived for fluid jets based on the surface area minimization principle. The quintessential work of Plateau-Rayleigh considers tiny perturbations (amplitude much less than the radius) to the continuous phase and for large amplitude perturbations, the breakup condition for the rod-shaped phase is still a knotty issue. Here, we present a concise thermodynamic model based on the surface area minimization principle as well as a non-linear stability analysis to generalize Plateau-Rayleigh’s criterion for finite amplitude perturbations. Our results demonstrate a breakup transition from a continuous phase via dispersed particles towards a uniform-radius cylinder, which has not been found previously, but is observed in our phase-field simulations. This new observation is attributed to a geometric constraint, which was overlooked in former studies. We anticipate that our results can provide further insights on microstructures with spherical particles and cylinder-shaped phases.
Electrolyte-gated transistors (EGTs) represent an interesting alternative to conventional dielectric-gating to reduce the required high supply voltage for printed electronic applications. Here, a type of ink-jet printable ion-gel is introduced and optimized to fabricate a chemically crosslinked ion-gel by self-assembled gelation, without additional crosslinking processes, e.g., UV-curing. For the self-assembled gelation, poly(vinyl alcohol) and poly(ethylene-alt-maleic anhydride) are used as the polymer backbone and chemical crosslinker, respectively, and 1-ethyl-3-methylimidazolium trifluoromethanesulfonate ([EMIM][OTf]) is utilized as an ionic species to ensure ionic conductivity. The as-synthesized ion-gel exhibits an ionic conductivity of ≈5 mS cm−1 and an effective capacitance of 5.4 µF cm−2 at 1 Hz. The ion-gel is successfully employed in EGTs with an indium oxide (In2O3) channel, which shows on/off-ratios of up to 1.3 × 106 and a subthreshold swing of 80.62 mV dec−1.
In the domain of printed electronics (PE), field-effect transistors (FETs) with an oxide semiconductor channel are very promising. In particular, the use of high gate-capacitance of the composite solid polymer electrolytes (CSPEs) as a gate-insulator ensures extremely low voltage requirements. Besides high gate capacitance, such CSPEs are proven to be easily printable, stable in air over wide temperature ranges, and possess high ion conductivity. These CSPEs can be sensitive to moisture, especially for high surface-to-volume ratio printed thin films. In this paper, we provide a comprehensive experimental study on the effect of humidity on CSPE-gated single transistors. At the circuit level, the performance of ring oscillators (ROs) has been compared for various humidity conditions. The experimental results of the electrolyte-gated FETs (EGFETs) demonstrate rather comparable currents between 30%-90% humidity levels. However, the shifted transistor parameters lead to a significant performance change of the RO frequency behavior. The study in this paper shows the need of an impermeable encapsulation for the CSPE-gated FETs to ensure identical performance at all humidity conditions.
Effective medium theories (EMT) are powerful tools to calculate sample averaged thermoelectric material properties of composite materials. However, averaging over the heterogeneous spatial distribution of the phases can lead to incorrect estimates of the thermoelectric transport properties and the figure of merit ZT in compositions close to the percolation threshold. This is particularly true when the phases’ electronic properties are rather distinct leading to pronounced percolation effects. The authors propose an alternative model to calculate the thermoelectric properties of multi‐phased materials that are based on an expanded nodal analysis of random resistor networks (RRN). This method conserves the information about the morphology of the individual phases, allowing the study of the current paths through the phases and the influence of heterogeneous charge transport and cluster formation on the effective material properties of the composite. The authors show that in composites with strongly differing phases close to the percolation threshold the thermoelectric properties and the ZT value are always dominated exclusively by one phase or the other and never by an average of both. For these compositions, the individual samples display properties vastly different from EMT predictions and can be exploited for an increased thermoelectric performance.
Electrolyte-gated, printed field-effect transistors exhibit high charge carrier densities in the channel and thus high on-currents at low operating voltages, allowing for the low-power operation of such devices. This behavior is due to the high area-specific capacitance of the device, in which the electrolyte takes the role of the dielectric layer of classical architectures. In this paper, we investigate intrinsic double-layer capacitances of ink-jet printed electrolyte-gated inorganic field-effect transistors in both in-plane and top-gate architectures by means of voltage-dependent impedance spectroscopy. By comparison with deembedding structures, we separate the intrinsic properties of the double-layer capacitance at the transistor channel from parasitic effects and deduce accurate estimates for the double-layer capacitance based on an equivalent circuit fitting. Based on these results, we have performed simulations of the electrolyte cutoff frequency as a function of electrolyte and gate resistances, showing that the top-gate architecture has the potential to reach the kilohertz regime with proper optimization of materials and printing process. Our findings additionally enable accurate modeling of the frequency-dependent capacitance of electrolyte/ion gel-gated devices as required in the small-signal analysis in the circuit simulation.
Hybrid low-voltage physical unclonable function based on inkjet-printed metal-oxide transistors
(2020)
Modern society is striving for digital connectivity that demands information security. As an emerging technology, printed electronics is a key enabler for novel device types with free form factors, customizability, and the potential for large-area fabrication while being seamlessly integrated into our everyday environment. At present, information security is mainly based on software algorithms that use pseudo random numbers. In this regard, hardware-intrinsic security primitives, such as physical unclonable functions, are very promising to provide inherent security features comparable to biometrical data. Device-specific, random intrinsic variations are exploited to generate unique secure identifiers. Here, we introduce a hybrid physical unclonable function, combining silicon and printed electronics technologies, based on metal oxide thin film devices. Our system exploits the inherent randomness of printed materials due to surface roughness, film morphology and the resulting electrical characteristics. The security primitive provides high intrinsic variation, is non-volatile, scalable and exhibits nearly ideal uniqueness.
A versatile liquid metal (LM) printing process enabling the fabrication of various fully printed devices such as intra- and interconnect wires, resistors, diodes, transistors, and basic circuit elements such as inverters which are process compatible with other digital printing and thin film structuring methods for integration is presented. For this, a glass capillary-based direct-write method for printing LMs such as eutectic gallium alloys, exploring the potential for fully printed LM-enabled devices is demonstrated. Examples for successful device fabrication include resistors, p–n diodes, and field effect transistors. The device functionality and easiness of one integrated fabrication flow shows that the potential of LM printing is far exceeding the use of interconnecting conventional electronic devices in printed electronics.
High-performance Ag–Se-based n-type printed thermoelectric (TE) materials suitable for room-temperature applications have been developed through a new and facile synthesis approach. A high magnitude of the Seebeck coefficient up to 220 μV K–1 and a TE power factor larger than 500 μW m–1 K–2 for an n-type printed film are achieved. A high figure-of-merit ZT ∼0.6 for a printed material has been found in the film with a low in-plane thermal conductivity κF of ∼0.30 W m–1 K–1. Using this material for n-type legs, a flexible folded TE generator (flexTEG) of 13 thermocouples has been fabricated. The open-circuit voltage of the flexTEG for temperature differences of ΔT = 30 and 110 K is found to be 71.1 and 181.4 mV, respectively. Consequently, very high maximum output power densities pmax of 6.6 and 321 μW cm–2 are estimated for the temperature difference of ΔT = 30 K and ΔT = 110 K, respectively. The flexTEG has been demonstrated by wearing it on the lower wrist, which resulted in an output voltage of ∼72.2 mV for ΔT ≈ 30 K. Our results pave the way for widespread use in wearable devices.
Oxide semiconductors are highly promising candidates for the most awaited, next-generation electronics, namely, printed electronics. As a fabrication route for the solution-processed/printed oxide semiconductors, photonic curing is becoming increasingly popular, as compared to the conventional thermal curing method; the former offers numerous advantages over the latter, such as low process temperatures and short exposure time and thereby, high throughput compatibility. Here, using dissimilar photonic curing concepts (UV–visible light and UV-laser), we demonstrate facile fabrication of high performance In2O3 field-effect transistors (FETs). Beside the processing related issues (temperature, time etc.), the other known limitation of oxide electronics is the lack of high performance p-type semiconductors, which can be bypassed using unipolar logics from high mobility n-type semiconductors alone. Interestingly, here we have found that our chosen distinct photonic curing methods can offer a large variation in threshold voltage, when they are fabricated from the same precursor ink. Consequently, both depletion and enhancement-mode devices have been achieved which can be used as the pull-up and pull-down transistors in unipolar inverters. The present device fabrication recipe demonstrates fast processing of low operation voltage, high performance FETs with large threshold voltage tunability.
Fully Printed Inverters using Metal‐Oxide Semiconductor and Graphene Passives on Flexible Substrates
(2020)
Printed and flexible metal‐oxide transistor technology has recently demonstrated great promise due to its high performance and robust mechanical stability. Herein, fully printed inverter structures using electrolyte‐gated oxide transistors on a flexible polyimide (PI) substrate are discussed in detail. Conductive graphene ink is printed as the passive structures and interconnects. The additive printed transistors on PI substrates show an on/off ratio of 106 and show mobilities similar to the state‐of‐the‐art printed transistors on rigid substrates. Printed meander structures of graphene are used as pull‐up resistances in a transistor–resistor logic to create fully printed inverters. The printed and flexible inverters show a signal gain of 3.5 and a propagation delay of 30 ms. These printed inverters are able to withstand a tensile strain of 1.5% following more than 200 cycles of mechanical bending. The stability of the electrical direct current (DC) properties has been observed over a period of 5 weeks. These oxide transistor‐based fully printed inverters are relevant for digital printing methods which could be implemented into roll‐to‐roll processes.
Amorphous In-Ga-Zn-O (IGZO) is a high-mobility semiconductor employed in modern thin-film transistors for displays and it is considered as a promising material for Schottky diode-based rectifiers. Properties of the electronic components based on IGZO strongly depend on the manufacturing parameters such as the oxygen partial pressure during IGZO sputtering and post-deposition thermal annealing. In this study, we investigate the combined effect of sputtering conditions of amorphous IGZO (In:Ga:Zn=1:1:1) and post-deposition thermal annealing on the properties of vertical thin-film Pt-IGZO-Cu Schottky diodes, and evaluated the applicability of the fabricated Schottky diodes for low-frequency half-wave rectifier circuits. The change of the oxygen content in the gas mixture from 1.64% to 6.25%, and post-deposition annealing is shown to increase the current rectification ratio from 10 5 to 10 7 at ±1 V, Schottky barrier height from 0.64 eV to 0.75 eV, and the ideality factor from 1.11 to 1.39. Half-wave rectifier circuits based on the fabricated Schottky diodes were simulated using parameters extracted from measured current-voltage and capacitance-voltage characteristics. The half-wave rectifier circuits were realized at 100 kHz and 300 kHz on as-fabricated Schottky diodes with active area of 200 μm × 200 μm, which is relevant for the near-field communication (125 kHz - 134 kHz), and provided the output voltage amplitude of 0.87 V for 2 V supply voltage. The simulation results matched with the measurement data, verifying the model accuracy for circuit level simulation.