Fine-Tuning the Performance of Ultraflexible Organic Complementary Circuits on a Single Substrate via a Nanoscale Interfacial Photochemical Reaction.

Flexible electronics has paved the way toward the development of next-generation wearable and implantable healthcare devices, including multimodal sensors. Integrating flexible circuits with transducers on a single substrate is desirable for processing vital signals. However, the trade-off between low power consumption and high operating speed is a major bottleneck. Organic thin-film transistors (OTFTs) are suitable for developing flexible circuits owing to their intrinsic flexibility and compatibility with the printing process. We used a photoreactive insulating polymer poly((±)endo,exo-bicyclo[2.2.1]hept-ene-2,3-dicarboxylic acid, diphenylester) (PNDPE) to modulate the power consumption and operating speed of ultraflexible organic circuits fabricated on a single substrate. The turn-on voltage (V on) of the p- and n-type OTFTs was controlled through a nanoscale interfacial photochemical reaction. The time-of-flight secondary ion mass spectrometry revealed the preferential occurrence of the PNDPE photochemical reaction in the vicinity of the semiconductor-dielectric interface. The power consumption and operating speed of the ultraflexible complementary inverters were tuned by a factor of 6 and 4, respectively. The minimum static power consumption was 30 ± 9 pW at transient and 4 ± 1 pW at standby. Furthermore, within the tuning range of the operating speed and at a supply voltage above 2.5 V, the minimum stage delay time was of the order of hundreds of microseconds. We demonstrated electromyogram measurements to emphasize the advantage of the nanoscale interfacial photochemical reaction. Our study suggests that a nanoscale interfacial photochemical reaction can be employed to develop imperceptible and wearable multimodal sensors with organic signal processing circuits that exhibit low power consumption.

Heterogeneous Functional Dielectric Patterns for Charge-Carrier Modulation in Ultraflexible Organic Integrated Circuits.

Flexible electronics have gained considerable attention for application in wearable devices. Organic transistors are potential candidates to develop flexible integrated circuits (ICs). A primary technique for maximizing their reliability, gain, and operation speed is the modulation of charge-carrier behavior in the respective transistors fabricated on the same substrate. In this work, heterogeneous functional dielectric patterns (HFDP) of ultrathin polymer gate dielectrics of poly((±)endo,exo-bicyclo[2.2.1]hept-ene-2,3-dicarboxylic acid, diphenylester) (PNDPE) are introduced. The HFDP that are obtained via the photo-Fries rearrangement by ultraviolet radiation in the homogeneous PNDPE provide a functional area for charge-carrier modulation. This leads to programmable threshold voltage control over a wide range (-1.5 to +0.2 V) in the transistors with a high patterning resolution, at 2 V operational voltage. The transistors also exhibit high operational stability over 140 days and under the bias-stress duration of 1800 s. With the HFDP, the performance metrics of ICs, for example, the noise margin and gain of the zero-VGS load inverters and the oscillation frequency of ring oscillators are improved to 80%, 1200, and 2.5 kHz, respectively, which are the highest among the previously reported zero-VGS -based organic circuits. The HFDP can be applied to much complex and ultraflexible ICs.

Heterogeneous Glioma Cell Invasion Under Interstitial Flow Depending on Their Differentiation Status.

Glioblastoma (GBM) is the most common and lethal type of malignant brain tumor. A deeper mechanistic understanding of the invasion of heterogeneous GBM cell populations is crucial to develop therapeutic strategies. A key regulator of GBM cell invasion is interstitial flow. However, the effect of an interstitial flow on the invasion of heterogeneous GBM cell populations composed of glioma initiating cells (GICs) and relatively differentiated progeny cells remains unclear. In the present study, we investigated how GICs invade three-dimensional (3D) hydrogels in response to an interstitial flow with respect to their differentiation status. Microfluidic culture systems were used to apply an interstitial flow to the cells migrating from the cell aggregates into the 3D hydrogel. Phase-contrast microscopy revealed that the invasion and protrusion formation of the GICs in differentiated cell conditions were significantly enhanced by a forward interstitial flow, whose direction was the same as that of the cell invasion, whereas those in stem cell conditions were not enhanced by the interstitial flow. The mechanism of flow-induced invasion was further investigated by focusing on differentiated cell conditions. Immunofluorescence images revealed that the expression of cell-extracellular matrix adhesion-associated molecules, such as integrin ß1, focal adhesion kinase, and phosphorylated Src, was upregulated in forward interstitial flow conditions. We then confirmed that cell invasion and protrusion formation were significantly inhibited by PP2, a Src inhibitor. Finally, we observed that the flow-induced cell invasion was preceded by nestin-positive immature GICs at the invasion front and followed by tubulin ß3-positive differentiated cells. Our findings provide insights into the development of novel therapeutic strategies to inhibit flow-induced glioma invasion. Impact statement A mechanistic understanding of heterogeneous glioblastoma cell invasion is crucial for developing therapeutic strategies. We observed that the invasion and protrusion formation of glioma initiating cells (GICs) were significantly enhanced by forward interstitial flow in differentiated cell conditions. The expression of integrin ß1, focal adhesion kinase, and phosphorylated Src was upregulated, and the flow-induced invasion was significantly inhibited by a Src inhibitor. The flow-induced heterogeneous cell invasion was preceded by nestin-positive GICs at the invasion front and followed by tubulin ß3-positive differentiated cells. Our findings provide insights into the development of novel therapeutic strategies to inhibit flow-induced glioma invasion.

Orientation analysis of pentacene molecules in organic field-effect transistor devices using polarization-dependent Raman spectroscopy.

Pentacene, an organic molecule, is a promising material for high-performance field effect transistors due to its high charge carrier mobility in comparison to usual semiconductors. However, the charge carrier mobility is strongly dependent on the molecular orientation of pentacene in the active layer of the device, which is hard to investigate using standard techniques in a real device. Raman scattering, on the other hand, is a high-resolution technique that is sensitive to the molecular orientation. In this work, we investigated the orientation distribution of pentacene molecules in actual transistor devices by polarization-dependent Raman spectroscopy and correlated these results with the performance of the device. This study can be utilized to understand the distribution of molecular orientation of pentacene in various electronic devices and thus would help in further improving their performances.

Ultralow-Noise Organic Transistors Based on Polymeric Gate Dielectrics with Self-Assembled Modifiers.

In this study, ultralow 1/f noise organic thin-film transistors (OTFTs) based on parylene gate dielectrics modified with triptycene (Trip) modifiers were fabricated. The fabricated OTFTs showed the lowest 1/f noise level among those of previously reported OTFTs. It is well known that 1/f noise causes degradation of signal integrity in analog and digital circuits. However, conventional OTFTs still possess high 1/f noise levels, and the factors that strongly affect 1/f noise are still ambiguous. In this work, the effect of gate dielectric surface on 1/f noise was investigated. First, by comparing OTFTs composed of various channel lengths, we revealed that contact resistance did not affect 1/f noise. Second, we compared parylene OTFTs with and without a self-assembled Trip modifier layer in terms of 1/f noise and trap density of states (Trap DOS). The experiments revealed that a specific Trip modifier layer suppresses the shallow Trap DOS in the OTFTs, leading to a low 1/f noise. Moreover, the 1/f noise level and Trap DOS of various kinds of OTFTs were comprehensively compared, which highlighted that the 1/f noise of OTFTs strongly depends on the gate dielectric surface. Finally, detailed analysis of the gate dielectric interface led us to conclude that the disorder of gate dielectrics and the crystalline quality of semiconductor films are related to shallow Trap DOS, which correlates with 1/f noise.

Raman Spectroscopic Studies of Dinaphthothienothiophene (DNTT).

The application of dinaphthothienothiophene (DNTT) molecules, a novel organic semiconductor material, has recently increased due to its high charge carrier mobility and thermal stability. Since the structural properties of DNTT molecules, such as the molecular density distribution and molecular orientations, significantly affect their charge carrier mobility in organic field-effect transistors devices, investigating these properties would be important. Here, we report Raman spectroscopic studies on DNTT in a transistor device, which was further analyzed by the density functional theory. We also show a perspective of this technique for orientation analysis of DNTT molecules within a transistor device.

Renewable Wood Pulp Paper Reactor with Hierarchical Micro/Nanopores for Continuous-Flow Nanocatalysis.

Continuous-flow nanocatalysis based on metal nanoparticle catalyst-anchored flow reactors has recently provided an excellent platform for effective chemical manufacturing. However, there has been limited progress in porous structure design and recycling systems for metal nanoparticle-anchored flow reactors to create more efficient and sustainable catalytic processes. In this study, traditional paper is used for a highly efficient, recyclable, and even renewable flow reactor by tailoring the ultrastructures of wood pulp. The "paper reactor" offers hierarchically interconnected micro- and nanoscale pores, which can act as convective-flow and rapid-diffusion channels, respectively, for efficient access of reactants to metal nanoparticle catalysts. In continuous-flow, aqueous, room-temperature catalytic reduction of 4-nitrophenol to 4-aminophenol, a gold nanoparticle (AuNP)-anchored paper reactor with hierarchical micro/nanopores provided higher reaction efficiency than state-of-the-art AuNP-anchored flow reactors. Inspired by traditional paper materials, successful recycling and renewal of AuNP-anchored paper reactors were also demonstrated while high reaction efficiency was maintained.

Antibacterial effect of bactericide immobilized in resin matrix.

OBJECTIVE: Biomaterials with anti-microbial properties are highly desirable in the oral cavity. Ideally, bactericidal molecules should be immobilized within the biomaterial to avoid unwanted side-effects against surrounding tissues. They may then however loose much of their antibacterial efficiency. The aim of this study was to investigate how much antibacterial effect an immobilized bactericidal molecule still has against oral bacteria. METHODS: Experimental resins containing 0, 1 and 3% cetylpyridinium chloride (CPC) were polymerized, and the bacteriostatic and bactericidal effects against Streptococcus mutans were determined. Adherent S. mutans on HAp was quantitatively determined using FE-SEM and living cells of S. mutans were quantified using real-time RT-PCR. The amount of CPC released from the 0%-, 1%- and 3%-CPC resin sample into water was spectrometrically quantified using a UV-vis recording spectrophotometer. RESULTS: UV spectrometry revealed that less than 0.11 ppm of CPC was released from the resin into water for all specimens, which is lower than the minimal concentration generally needed to inhibit biofilm formation. Growth of S. mutans was significantly inhibited on the surface of the 3%-CPC-containing resin coating, although no inhibitory effect was observed on bacteria that were not in contact with its surface. When immersed in water, the antibacterial capability of 3%-CPC resin lasted for 7 days, as compared to resin that did not contain CPC. SIGNIFICANCE: These results demonstrated that the bactericidal molecule still possessed significant contact bacteriostatic activity when it was immobilized in the resin matrix.

Gene profiles during root canal treatment in experimental rat periapical lesions.

The purpose of this study was to profile gene expression in periapical lesions during root canal treatment (RCT). Periapical lesions were induced experimentally by exposing the pulp in Sprague-Dawley rats. After 3 wk, the animals received root canal filling (RCF) and were sacrificed 1 or 4 wk later. From the periapical tissues, total RNA was extracted and processed for cDNA-microarray analysis. The lesions were histologically and radiographically confirmed to expand 4 wk after pulp exposure (inflammation phase) and to stabilize 4 wk after RCF (healing phase). In approximately 30,000 genes on the microarray, 203 genes were up-regulated to more than 5-fold (e.g., IL-1beta), and 864 genes were down-regulated to less than 20% of baseline level (e.g., caspase 8) in inflammation phase. Compared with inflammation phase, we found that 133 genes were up-regulated (e.g., IL-1alpha) and 50 genes were down-regulated (e.g., defensin alpha5) in healing phase. Corresponding to the gene expression profiles, accumulation of IL-1alpha and IL-1beta was observed in the periapical lesions by immunohistochemistry. These gene profiles might be useful in diagnosing the healing process of periapical lesions.