A platform for high-bandwidth nanopore sensing with thermal control and low electrical noise.

Effect of single nanoparticle-nanopore interaction strength on ionic current modulation

Solid-state nanopores have been widely used in the detection of biomolecules, but improving DNA sequencing resolution remains a significant challenge. Polyacrylic acid (PAA), known for its abundant carboxyl groups and excellent hydrophilicity, emerges as an ideal material for nanopore sensors. This study, based on molecular dynamics simulations, demonstrates that nanopore sensors incorporating PAA exhibit a "braking" effect. This effect slows down the translocation speed of single-stranded DNA (ssDNA) while enhancing its recognition capability. Findings reveal that a 15% mass fraction of PAA with a polymerization degree of 60 increases the dwell time of ssDNA by approximately 21-fold. In contrast, a 30% mass fraction of PAA with a polymerization degree of 15 extends the ssDNA dwell time by about 30-fold. The addition of a 20% mass fraction PAA with a polymerization degree of 15 significantly increased the dwell times of all ssDNA sequences, with poly(dG)20 showing a notable 20-fold increase. Moreover, the relative current blockage surpassed 0.5 for all ssDNA sequences, with significant variations observed among different sequences. As the polymerization degree or mass fraction of PAA increases, enhanced electrostatic and van der Waals interactions with ssDNA, along with increased hydrogen bond formation, prolong the ssDNA dwell time. Our research demonstrates that PAA effectively enhances the resolution of nanopore DNA sequencing, providing novel insights for developing high-performance nanopore sensors.

The influence of penetrating radiations on the electrical low-frequency noise of semiconductors is studied. Expression is calculated that determines the number of structural defects in semiconductors arising from exposure to penetrating radia-tion. General form expression is calculated for the spectrum of electrical low-frequency noise in semiconductors when exposed to penetrating radiation. Quanti-tative relationship was established between the spectrum of electrical low-frequency noise and the development of disturbances in the structure of semicon-ductors caused by penetrating radiations. The results obtained can be used to de-termine the spectra of electrical noise in semiconductors of various types and in numerous semiconductor devices. The results of the article have practical applica-tions. Calculated expressions allow to make estimates of the intensity of electrical low-frequency noise, from which conclusions can be drawn about possibility of functioning and reliability of semiconductor devices. Established relationship be-tween electrical noise and radiation defects can be used to estimate, based on spec-tral characteristics of the noise, the defectiveness of structure of semiconductors subjected to radiation damage.

Solid-state nanopore sensors are highly versatile platforms for the rapid, label-free electrical detection and analysis of single molecules, applicable to next generation DNA sequencing. The versatility of this technology allows for both large scale device integration and interfacing with biological systems. Here we report on the development of a hybrid biological solid-state nanopore platform that incorporates a highly mobile lipid bilayer on a single solid-state Al(2)O(3) nanopore sensor, for the potential reconstitution of ion channels and biological nanopores. Such a system seeks to combine the superior electrical, thermal, and mechanical stability of Al(2)O(3) solid-state nanopores with the chemical specificity of biological nanopores. Bilayers on Al(2)O(3) exhibit higher diffusivity than those formed on TiO(2) and SiO(2) substrates, attributed to the presence of a thick hydration layer on Al(2)O(3), a key requirement to preserving the biological functionality of reconstituted membrane proteins. Molecular dynamics simulations demonstrate that the electrostatic repulsion between the dipole of the DOPC headgroup and the positively charged Al(2)O(3) surface may be responsible for the enhanced thickness of this hydration layer. Lipid bilayer coated Al(2)O(3) nanopore sensors exhibit excellent electrical properties and enhanced mechanical stability (GΩ seals for over 50 h), making this technology ideal for use in ion channel electrophysiology, the screening of ion channel active drugs and future integration with biological nanopores such as α-hemolysin and MspA for rapid single molecule DNA sequencing. This technology can find broad application in bio-nanotechnology.

Low frequency electrical and optical noise fluctuations of organic light emitting diodes were obtained simultaneously. It had been observed that the voltage and optical noises increased gradually with time as the device was subjected to constant current stress. Correlation between the device electrical and optical noise was established. Computation of the correlation coefficients between the voltage and luminescence noises had been devised and implemented. Results suggested that the correlation increased with the noise frequency and this phenomenon was concluded to be the result of some photons going undetected at low frequencies. It was further observed that the correlation was more consistent under low device current when the current efficiency was higher.

Nanopores have recently emerged as high-throughput tools for probing and manipulating nucleic acid secondary structure at the single-molecule level. While most studies to date have utilized protein pores embedded in lipid bilayers, solid-state nanopores offer many practical advantages which greatly expand the range of applications in life sciences and biotechnology. Using sub-2 nm solid-state nanopores, we show for the first time that the unzipping kinetics of individual DNA duplexes can be probed by analyzing the dwell-time distributions. We performed high-bandwidth electrical measurements of DNA duplex unzipping as a function of their length, sequence, and temperature. We find that our longer duplexes (>10 bp) follow Arrhenius dependence on temperature, suggesting that unzipping can be approximated as a single-barrier crossing, but the unzipping kinetics of shorter duplexes do not involve a barrier, due to the strong biasing electrical force. Finally, we show that mismatches in the duplex affect unzipping times in a position-sensitive manner. Our results are a crucial step toward sequence variability detection and our single-molecule nanopore sequencing technology, which rely on parallel detection from nanopore arrays.

The dynamic structural behavior in DNA due to interaction with cisplatin is essential for the functionality of platinum-based anti-cancer drugs. Here we report a novel method to monitor the interaction progress in DNA-cisplatin reaction in real time with a solid-state nanopore. The interaction processes are found to be well elucidated by the evolution of the capture rate of DNA-cisplatin complex, which is defined as the number of their translocation events through the nanopore in unit time. In the first stage, the capture rate decreases rapidly due to DNA discharging as the positive-charged hydrated cisplatin molecules initially bond to the negative-charged DNA and form mono-adducts. In the second stage, by forming di-adducts, the capture rate increases as DNA molecules are softened, appears as the reduced persistence length of the DNA-cisplatin adducts. In the third stage, the capture rate decreases again as a result of DNA aggregation. Our study demonstrates a new single-molecule tool in exploring dynamic behaviors during drug-DNA reactions and may have future application in fast drug screening.

The influence of parasitic elements on the wide-band electrical noise in GaAlAs BH-BOG lasers is investigated theoretically and experimentally. The results show that the maximum small-signal modulation bandwidth can be determined from measurements of the electrical noise spectrum. A small difference of the peak frequency in the optical intensity noise and the peak frequency in the electrical noise spectra is observed (about 200 MHz), and it is explained by introducing the nonlinear intrinsic diode impedance in the parasitic element model. However, the peak frequency in the small-signal modulation response spectrum coincides with the peak frequency in the electrical noise spectrum. It is also shown that the spectral line width, calculated from electrical noise measurements, is not significantly affected by the parasitic element filtering. The electrical noise level is observed to approach an inverse output power dependence at high pumping rates, in good agreement with theoretical calculations.

A solid electrolyte detector for the determination of trace amounts of oxygen in the presence of argon and other gases

Because the piezoelectric fast steering mirror (PFSM) typically has fast response speed, high resolution, low energy consumption, and low electrical noise, it plays a crucial role in precision tracking systems for laser communication. However, accurately describing the dynamical behaviour of the PFSM is challenging due to the existence of hysteresis. Therefore, this study explores modeling algorithms for PFSM system based on the Koopman operator. We primarily construct the Deep-Koopman architecture, utilizing a two-layer deep neural network (DNN) instead of manually selecting basis functions. This maps the system state to a high-dimensional space and represents the evolution trajectory of PFSM system based on the linear representation of the Koopman operator, which is more precise compared to the model solved based on extended dynamic mode decomposition (EDMD). By incorporating time-delay embedding to process the original sampled sequences, the prediction accuracy is further improved, leading to the delay-deep Koopmam model. Its effectiveness and advantage have been verified through experiments.

Solid-state nanopores are nm sized apertures formed in thin synthetic membranes. These single molecule sensors have been used in a variety of biophysical and diagnostic applications and serve as a potential candidate in the development of cost-effective, next generation DNA sequencing technologies, critical to furthering our understanding of inheritance, individuality, disease and evolution. The versatility of solid-state nanopore technology allows for both interfacing with biological systems at the nano-scale as well as large scale VLSI integration promising reliable, affordable, mass producible biosensors with single molecule sensing capabilities. In addition, this technology allows for truly parallel, high throughput DNA and protein analysis through the development of nanopore and micropore arrays in ultra-thin synthetic membranes. This chapter is focused on the development of solid-state nanopore sensors in synthetic membranes and the potential benefits and challenges associated with this technology. Biological nanopores, primarily α-hemolysin and the phi29 connector are also reviewed. We conclude with a detailed discussion on chemically modified solid-state nanopores. These surface functionalized nanopore sensors combine the stability and versatility of solid-state nanopores with the sensitivity and selectivity of biological nanopore systems and may play an important role in drug screening and medical diagnostics.Keywordsα-hemolysinphi29Nanopores in Al2O3 MembranesSurface Charges in NanoporesSurface Enhanced DNA Transport

Nanopore sensors have attracted considerable interest for high-throughput sensing of individual nucleic acids and proteins without the need for chemical labels or complex optics. A prevailing problem in nanopore applications is that the transport kinetics of single biomolecules are often faster than the measurement time resolution. Methods to slow down biomolecular transport can be troublesome and are at odds with the natural goal of high-throughput sensing. Here we introduce a low-noise measurement platform that integrates a complementary metal-oxide semiconductor (CMOS) preamplifier with solid-state nanopores in thin silicon nitride membranes. With this platform we achieved a signal-to-noise ratio exceeding five at a bandwidth of 1 MHz, which to our knowledge is the highest bandwidth nanopore recording to date. We demonstrate transient signals as brief as 1 μs from short DNA molecules as well as current signatures during molecular passage events that shed light on submolecular DNA configurations in small nanopores.

Protein detection and identification at the single-molecule level are major challenges in many biotechnological fields. Solid-state nanopores have raised attention as label-free biosensors with high sensitivity. Here, we use solid-state nanopore sensing to discriminate two closely related proteins, α-thrombin and γ-thrombin. We show that aptamer functionalization improves protein discrimination thanks to a significant difference in the relative current blockade amplitude. To enhance discrimination, we postprocessed the signals using machine learning and training algorithms and we were able to reach an accuracy of 98.8% using seven features and ensemble methods.

ABSTRACTNanopore-based sensor is a new single-molecule level sensing method, which involves detecting the currentchange and translocation time of the molecule when it passes through the pore by the electrophoresis. In thiswork, the lambda-DNA was driven thread through the solid-state nanopore of different diameters to characterizeDNA’s physical properties from its translocation process in 1 M KCl salt solution. Firstly, the frequency of eventsincreased with the rising voltages. We found that the event frequency for 200 mV decreased because of thereduced concentration of the -DNA after about two hours’ translocation process under other voltages. Andthe duration times of lambda-DNA translocation events which linearly passed through the nanopore at differentvoltages were analyzed with the “rst-passage-time distribution indicated that the electrophoretic mobility oflambda-DNA is 1.153× 10 Š 10 m 2 V Š 1 s Š 1 under the condition of 1 M KCl buffer and 22 nm nanopore. Besides,we investigated two methods to calculate the diffusion constant D. The two results agreed with each otherquite well. The capture rate increased with the voltage at a “xed DNA concentration. The data analysis of DNApassing through nanopores with different sizes suggested that the diameter of the nanopore plays a key factorin DNA translocation behavior. This is an important result for the label-free sensing by solid-state nanopore inthe future and will provide more evidences for the development of nanopores as a multi-functional sensor for awide range of biopolymers and nanoparticles.KEYWORDS: Solid-State Nanopore, Double-Strand DNA, Translocation Time, Current Blockage,Electrophoretic Mobility, Diffusion Constant.

An ultra-thin natural-source-based cellulose derivate is used in a bilayer gate dielectric for organic complementary inverters. Extraordinarily high small-signal gains up to 1600, a very sharp transition region (as low as 40 mV), a full rail-to-rail swing, a balanced noise margin of 92.5%, and “long-time” stability are shown, revealing that these inverters are highly suitable for complex circuit designs. For more than a decade now the research in organic electronics was driven by unique consumer markets demanding for electronic circuits on flexible substrates over large areas and ideally at low cost. Meanwhile, versatile macroelectronic applications with attractive form factors such as flexible displays,1-4 large-area sensor arrays,5-11 e-paper,12, 13 low-cost radio-frequency identification tags,14-18 and bendable microprocessors19 have been realized using organic thin-film transistors (OTFTs) as the essential element. In the majority of these applications OTFTs are integrated either in the form of arrays or as digital logic. The fundamental building block of digital logic is the inverter, a circuit that inverts an input signal. Much work has been devoted in the last five years to design unipolar inverters using p-type-only OTFTs.18-23 Unfortunately, unipolar logic based on single gate OTFTs always suffers from high power consumption and low noise margin coupled with high noise margin variability and therefore impedes the fabrication of complex circuits having hundreds or more logic gates.19, 22, 23 In this context, it stands beyond doubt that the integration of both n-type and p-type transistors in complementary organic-based circuits12 is very advantageous due to a lower power dissipation, higher noise margin, better operational stability, and easier design of the circuit.24-27 To date, several major obstacles complicated the development of organic complementary circuits, which are as follows: i) the lack of n-channel OTFTs with a performance comparable to the p-channel OTFTs, ii) the challenge of device stability (difficulty in fabricating OTFTs with hysteresis-free characteristics), and iii) the difficulty in fabricating sufficiently thin gate dielectrics allowing for low supply voltages. Although many recently reported complementary organic inverters are impressive with respect to their low operation voltages (≤5 V),27-36 high static gains (>100 V/V),25, 28, 30, 32 and large noise margins (>80%),25, 35, 37, 38 only few of those can combine low-voltage operation with high gain and sufficient immunity against electrical noise.39 Moreover, there have been few investigations of the influence of hysteresis and threshold voltage shifts on the inverter characteristics, which typically gives rise to electrical instabilities and performance limitations of those devices.32, 39 The inverter's noise margin is the most critical parameter, since it directly determines the maximum complexity of circuits.22 Particularly, interesting applications of organic electronic circuits are found in analog electronics that allow for the read-out and processing of signals from printed large-area sensors and form an interface to silicon electronics. Examples are analog-to-digital (A/D) converters, operational amplifiers, and comparators, all including several tens of transistors, thus requiring both high gain and a large noise margin to be functional as well as sufficient processability. It is interesting to note that the majority of organic complementary inverters already mentioned24-34, 36-40 relied on pentacene as the p-type semiconductor (14 incidences), fluorinated copper phthalocyanine (6 incidences), or N,N′-ditridecylperylene-3,4,9,10-tetracarboxylic diimide (5 incidences) as the n-type material. On the contrary, the variation in gate dielectric materials that are used is much higher with an emphasis on hybrid dielectric systems. Hybrid systems allow accounting for both a high dielectric breakdown voltage and an engineered interface to the semiconductor. Moreover, the implementation of biodegradable and biocompatible materials represents a new niche in the organic electronics research, aimed to address the issues of cost and toxicity to humans and environment posed by nowadays electronics, a topic that was recently reviewed elsewhere.41-43 Accordingly, we have demonstrated the usage of a novel hybrid and biodegradable high-k gate dielectric material system based on a cellulose derivative for low-voltage complementary organic circuits with exceptional high noise margins.35 Previous work done in our laboratories demonstrated the fabrication feasibility of complex circuits, where the electrode patterning was performed by a self-aligned photolithography technique.44, 45 This process can easily be transferred to an anodized aluminum (Al2O3) + trimethylsilyl cellulose (TMSC) based bilayer system; the respective results will be published soon. To follow on this preliminary work we have developed an extraordinarily well-performing complementary inverter technology based on a hybrid dielectric composed of a bilayer of alumina (Al2O3) and trimethylsilyl cellulose (TMSC) and pentacene or C60 for the p-channel and the n-channel organic semiconductor, respectively. It outperforms any inverter reported so far with respect to the combination of excellent key parameters, such as record DC gain of above 500 V/V, low operation voltage of only 4 V, and large noise margin up to 92.5%. In order to clarify the origin for this high performance, special attention is given to the investigation of the semiconductor–dielectric interface, the semiconductor morphology, the nature of traps, the influence of mobility levels on the inverter performance and its long-term stability. This article is not meant to report new materials and systems, but rather find explanations and present a thorough analysis of the extraordinary performance of the cellulose derivative (TMSC) dielectric and the TMSC to semiconductor interface in organic field-effect transistors and simple inverter circuits. All OTFTs presented in this work have a bottom gate, top contact device architecture, as illustrated in Figure 1a. The transistor fabrication process is described in detail in the Experimental Section. The semiconducting layer is pentacene for p-type and C60 (fullerene) for n-type conduction. For the gate dielectric, an inorganic (Al2O3)–organic (TMSC) bilayer is chosen with 28 and 30 nm layer thickness, respectively. The dielectric properties of both single-layer TMSC films and bilayer Al2O3 + TMSC films, were investigated by current–voltage (I(V)), capacitance–frequency (C(f)), and capacitance–voltage (C(V)) measurements in appropriate capacitor structures with 72 nm insulator layer thickness of pure TMSC and 28 + 30 nm of bilayer film of Al2O3 + TMSC, respectively. In Figure 1b, the I(V) curves of a representative capacitor formed by a single layer cellulose dielectric is shown, whereas in Figure S1a (in the Supporting Information) the curve with bilayer dielectric is displayed. A comparison of I(V) curves of a single layer and bilayer dielectric is displayed in Figure 1c. At an electric field of 3.0 MV cm−1 (equivalent to ≈22 V) a current density on the order of 10−6 A cm−2 is observed for the single-layer TMSC. A breakdown field of 4.5 ± 0.3 MV cm−1 is extracted from eight appropriate capacitor structures. One representative C(V) measurement is displayed in Figure 1d. Its capacitance of about 29 nF cm−2 corresponds to a dielectric constant of εR = 2.4 ± 0.2 at 1 kHz with an excellent stability at frequencies down to 0.5 mHz (virtually flat dielectric constant and low dielectric losses which are indicative of a high purity and negligible amount of mobile ionic species) as illustrated in Figure 1e.46 In comparison, capacitors based on the bilayer dielectric have three orders of magnitude lower leakage currents (≈10−9 A cm−2) at an electric field of 3.0 MV cm−1 corresponding to ≈17.5 V and an effective capacitance of 53 nF cm−2 at 1 kHz (see Figure S1a,b, Supporting Information). As can be derived from Figure S1c (in the Supporting Information) the permittivity of the bilayer dielectric also shows excellent stability over the tested frequency range (1 mHz to 10 kHz). The measured capacitance value of the dielectric is in good agreement with calculations by assuming a permittivity of 9 and a thickness of 28 nm for the Al2O3 layer as well as a measured permittivity of 2.4 ± 0.2 (Figure 1e) and 30 nm thickness for the TMSC layer (see the Experimental Section). In any OTFT with bottom gate architecture the surface properties of the gate dielectric (surface energy, surface roughness) decisively affect the arrangement and growth of small molecule semiconductors. The surface energy of spin-coated TMSC thin films was determined by contact angle measurements. With a water contact angle of 98.5°, TMSC can be regarded as a hydrophobic, low energy surface material with a total surface energy of γ = 24.2 ± 0.6 mN m−1, separable in a small polar component γP = 1.8 ± 0.5 mN m−1 and a dispersive component γD = 22.4 ± 0.1 mN m−1. The average surface roughness, indicated by the root mean square (rms)–roughness values, was found to be only 0.77 ± 0.1 nm by atomic force microscopy (AFM) measurements. On this smooth and low energy TMSC surface, a small-grain growth mode with average grain sizes between 150 and 300 nm for pentacene (shown in Figure 1a) and 50 nm for C60 was observed by AFM measurements. In Figure 2, typical electrical characteristics of OTFTs with either C60 or pentacene as the semiconducting layer are plotted. Both p- and n-type transistors are based on the inorganic–organic bilayer gate dielectric composed of Al2O3 and TMSC. The output characteristics ID(VDS) are displayed in Figure 2a,b, whereas the transfer characteristics ID(VGS) are shown in Figure 2c,d. Both transistor types display very small hysteresis between forward and reverse voltage sweeps. The output characteristics show clear saturation, but for the pentacene-based OTFT a non-linear behavior of the drain current at very low drain voltages is observable (Figure 2b). Such an S-shape of the output curve has been already observed and reported for many different device configurations and has sometimes been attributed to a lateral field dependent contact resistance.47-55 In Table 1, the critical device parameters Von (onset voltage), Vthr (threshold voltage), S (subthreshold swing), μlin (charge carrier mobility in the linear regime), and μsat (charge carrier mobility in the saturation regime) are compiled and averaged over eight devices for each transistor type. On average, C60-based OTFTs show a charge carrier mobility of 0.7 cm2 V−1 s−1 in the saturation regime, a threshold voltage of 1.3 V, and a small subthreshold swing of 305 mV dec−1. Pentacene-based OTFTs have on average a mean threshold voltage of −4.7 V, a very small subthreshold swing of 225 mV dec−1, and a field-effect mobility of 0.22 cm2 V−1 s−1 in the saturation regime. The gate leakage currents are very low and in the range of 10−10 A. The balanced performance of our p- and n-type OTFTs, as well as the fact that both transistor types strictly behave as normally off transistors at zero applied gate voltage is a good base for integrating them in complementary organic inverters. A schematic image of such a complementary inverter circuit is displayed in Figure 3a together with the voltage transfer characteristics (VTCs) of a typical device and the static gain measured for operation voltages of VDD = 4, 5, 6, and 7 V. The inverter exhibits extraordinarily high small-signal gains; for all operation voltages, gains above 500 V/V are measured with a maximum value of about 1000 V/V for VDD = 7 V. The best performing device even has a maximum gain value of 1600 V/V. Moreover, a very sharp transition regime (ΔVin ≤ 40 mV) and a full rail-to-rail swing are observed. The extracted inverter parameters are compiled in Table 2. The switching threshold voltages VM are found to be very close to the ideal value of VDD/2 at all operation voltages with a nearly perfect fit (e.g., VM = 2.04 V at VDD = 4 V). In Figure 3b, the mismatches of the threshold voltages to the ideal values (ΔVM) are plotted as a function of VDD revealing a linear increase of ΔVM with the supply voltage. This means that the asymmetry of the VTCs increase with increasing the operation voltages. Additionally, the noise margins (NM) are plotted in Figure 3b as a function of VDD, illustrating the linear decrease of the NM with increasing operation voltage. Such a behavior reveals the direct correlation between ΔVM and NM and is an indication of the deviation of the VTCs from perfect symmetry. The noise margin is an important figure of merit of an inverter stage and measures the immunity against inevitable transistor parameter variations and electrical noise.56 There are several ways to determine the noise margin of an inverter. One convenient way is called the “maximum equal criterion” (MEC), where the NM is found by the maximum square that fits between inverter transition curve and the mirrored inverter curve as shown in Figure 3c.22, 35 The NM values for all the supplied voltages are listed in Table 2. The noise margin is mainly limited by the steepness of the transition ΔVin and the position of the switching threshold voltage VM (VM = Vin = Vout) as shown in Figure 3c. High and balanced noise margins are found when the ideal condition VM = VDD/2 is met, thus when VM = Vin =VDD/2 = Vout. The inverter in Figure 3c has a NM of 1.79, which is 90% of the maximum theoretical value for a supply voltage of 4 V, determined by the “maximum equal criterion.” Additionally, the “negative slope criteria” reveals a balanced NM of 1.85 V (92.5%) for a supply voltage of 4 V. The OTFTs with pentacene and C60 semiconductor layers (as used in the complementary inverters) were also analyzed with regard to their long-term stability. The dependence of their onset voltage and charge carrier mobility on the time period after preparation is plotted in Figure 4 based on measurements of at least five devices for each transistor type. The error bars display the standard deviations. p- and n-type devices exhibit an onset voltage shift of +1.3 and +0.95 V, respectively, over a period of 45 days. The main part of the shift occurred either after the first or after the second measurement and then the onset voltage shift tended to saturate. It seems that both pentacene- and fullerene-based devices stabilized their electrical properties after few days. Between day 8 and day 45 no significant change in the transfer characteristics was observed. Concerning the subthreshold swing, no significant change was observed over 45 days (S = 215 mV dec−1 (0 days), 210 mV dec−1 (8 days), and 225 mV dec−1 (45 days)) in the pentacene OTFTs, indicating that the interface trap density is stable. On the contrary, after 8 days an increase of the swing was observed for the C60 devices from 305 mV dec−1 (0 days), to 410 mV dec−1 (8 days), to 430 mV dec−1 (45 days). The mean value of the charge carrier mobility of the pentacene OTFTs showed no significant variation over 45 days: 0.22 cm2 V−1 s−1(fresh sample), 0.19 cm2 V−1 s−1 (after 8 days), 0.21 cm2 V−1 s−1 (after 45 days). In contrast, a strong reduction of about one order of magnitude (from 0.7 to 0.06 cm2 V−1 s−1 within the first 8 days and to 0.05 cm2 V−1 s−1 after 45 days) was observed for the fullerene transistors. In order to test the reliability of our OTFT devices we have also performed negative and positive bias stress tests. The bias stress was done 1 day after fabrication, on devices which had been previously measured only once. A reversible negative onset voltage shift of about 400 mV was observed under negative bias of −7.5 V over 21 hours stress (see Figure 5a,b) The main part of the negative voltage shift occurred during the first 2 hours (300 mV) whereas shift saturation was reached after 6 hours. The positive bias stress resulted in a significantly smaller positive onset voltage shift (ca. +100 mV over 4 hours stressing the device). Devices that were stored for seven months in the glovebox showed no bias stress effect at all (i.e., shift of the onset voltage) when their transistor characteristics were measured at regular intervals during the storage period. In order to investigate the “long-time” behavior of complementary inverters, electrical measurements were done after 1, 4, 8, and 45 days of the respective device preparation. Inverters were measured 1 day after device stabilization (see Figure 4a,b). The “long-time” behavior of complementary inverters is shown in Figure 4c,d where the VTC and gain curves are plotted as a function of time. For the lowest VDD of only 4 V, a small shift of the switching threshold voltage was measured: starting from 2.04 V after 1 day to an identical value of 2.17 V after 8 and 45 days, respectively, with a related exceptional high noise margin of 1.79 V (90% of the theoretical maximum) after 1 day and 1.74 V (87%) after 8 and 45 days. It is interesting to note that, after 8 days of storage time, the hysteresis in inverter characteristics was virtually negligible (<100 mV, see Figure 4d) and moreover, repeated measurements did not change the inverter transition, although the gain was somewhat reduced (from 503 (0 days) to 320 (8 days) and 195 (45 days)). The operational stability of the VTC was shown over a period of at least 45 days (Figure 4c for VDD = 4 V). Furthermore, the remarkable long-term stability of these TMSC-based complementary inverters was demonstrated by 16 consecutively recorded inverter curves that are virtually superimposed over one another (Figure 5c). The current–voltage characteristics show that the Al2O3 + TMSC bilayer capacitors have substantially lower leakage currents than the single TMSC layer devices. Due to the roughness of the aluminum bottom electrode with spikes up to 10 nm, the anodization process is a convenient method to reduce the leakage currents for at least three orders of magnitude at an electric field of 3 MV cm−1 as displayed in Figure 1d and make the dielectric layer more robust.57 Another advantage of the anodization step is the substitution of the hydroxide of the native oxide layer. Finally, the subsequent short oxygen plasma treatment (see the Experimental Section) is sufficiently removing all residuals left after the anodization process. This procedure allows for the generation of a pure and trap-reduced dielectric interface to the organic semiconductors, by measurements at low revealing a virtually flat permittivity in the mHz to kHz frequency range and low dielectric losses which both are indicative of a high purity and negligible amount of mobile ionic The generation of this excellent interface is in virtually hysteresis-free characteristics of all the One important that the performance of OTFTs, and in the charge carrier is the of the As shown by several the of the surface energy of the to that of the is one important the growth For a low surface energy material with a smooth surface TMSC, a growth mode is and with a rather high density and small grain sizes are formed (see Figure The high density of grain a significant decrease of the charge carrier since grain as charge On the a better between pentacene on low surface energy materials TMSC with and better reduce the of trap thus the mobility of charge in the In there is an between grain related and interface with regard to their influence on charge carrier The low subthreshold swing observed in all our pentacene-based OTFTs is indicative of a low interface trap density which the influence of the large grain trap density on the charge carrier Accordingly, a mobility 0.2 cm2 V−1 s−1 is observed in the p-type devices. In C60 films, the influence of on the charge carrier mobility is by far not as significant as in pentacene films, which is attributed to the of the fullerene In the pentacene OTFTs (see Figure a non-linear current increase in the linear regime of the ID(VDS) output characteristics is at higher gate have been in to such a which can be observed in bottom gate The explanations i) the of the charge carrier mobility for semiconductor ii) currents that the of the mobile by an effective under the drain and iii) large at the electrode from an energy between the work of contact material and semiconductor films, a gate or large contact are found in our of these it has been shown that a mobility in combination with a small contact in a non-linear drain voltage dependence of the current due to The from a of from trap and a dependence of on the drain A respective of the pentacene output curve in Figure the dependence in the regime 2 V, thus indicating that a mobility has to be The of any hysteresis in the I(V) curves and the low and value of the subthreshold swing a low density of interface in the pentacene are not for the observed and the of the as by the of the pentacene layer gives rise to which to a field dependence of the charge carrier This is all the more given that the pentacene grain sizes are 300 nm at a large density of grain As by Figure 4 the characteristics of both pentacene- and C60-based OTFTs show a positive onset voltage shifts storage which after a of measurements. The virtually subthreshold swing in pentacene as well as the negligible hysteresis as the origin of the On the contrary, it seems that trap are for the positive onset voltage shift in are either over time or during the first measurements by the applied positive gate be easily by the gate bias and therefore are not to the swing, but the small onset voltage in pentacene-based It has been reported by many that the of the of trap in pentacene trap also be due to such as at the a at the or a at the fabrication and transfer from the to the measurement stage the semiconductor layer and rise to such For oxygen can even the devices are to but transferred directly and measured in a glovebox with reduced oxygen and water have also observed that the of oxygen with pentacene is in the that these are under device operation with the of oxygen in the grain observed that the storage of devices in and their subsequent measurement in did not a change in their I(V) also observed that the storage time to the first measurement has influence on the device (i.e., on the onset voltage in this of and the first measurement the of to the of oxygen or with the which in a second are by Moreover, also are are not as in the as the (see and This an for the positive shift of the onset voltage between first and second measurement (Figure and also for the saturation of the onset voltage shift in In order to clarify which of are present in our we performed measurements on pentacene films (in and after storage in for (see Figure Supporting Information). storage under a small increase of the at energy is observed that can be attributed to the to and The analysis reveals an increase of the from 0.2 to At the position no change is that trap in our devices for bias stress and the positive onset voltage can mainly be attributed to It be that the of any mobility in pentacene OTFTs against an of pentacene both are to oxygen For the C60 transistors, one a strong decrease of the charge carrier mobility during 8 days of storage which is by all over the device grain This is a effect of The decrease in charge carrier mobility and the at the interface that the subthreshold swing is in a positive onset voltage shift of the C60 transistors. With respect to the complementary inverters, noise margin values beyond from the maximum theoretical value for all supply voltages are and the high operational of the OTFT devices. At a very low supply voltage of 4 V, our bilayer organic complementary inverters have a static gain of more than 500 V/V with a noise margin of 92.5%, which is already reported devices with architecture (see the of inverter performance given in 38 and also gain values above 1000 V/V values up to 1600 were measured for our devices. This is all the most as the charge carrier mobility values of the transistors are not thus the that the of the mobility values between p- and n-channel with the virtually hysteresis are the factors for high gain and high noise margin Accordingly, a mobility 1 be the the is not high ≤ it can be by and p-channel transistors with different In our the mobility is The static of a complementary inverter is determined by technology parameters, the parameters of p- and n-type transistors. A good of these parameters a good saturation of both output can to a significant increase of the gain A is shown in the Supporting Furthermore, high gain values are also determined by the interface An insulator with an low trap density (as this is the for is in having I(V) curves with virtually zero Accordingly, it is to measurements with a very high voltage small voltage thus one to the high gain value of the complementary inverter it by hysteresis The noise margin with increasing VDD due to their strong this is also for the of the VTCs by see Figure A for this behavior can be found in the bias stress that was observed for both types of transistors. The negative shift of Von under negative gate and the positive