3D printable and biocompatible PEDOT:PSS-ionic liquid colloids with high conductivity for rapid on-demand fabrication of 3D bioelectronics.

3D printing has been widely used for on-demand prototyping of complex three-dimensional structures. In biomedical applications, PEDOT:PSS has emerged as a promising material in versatile bioelectronics due to its tissue-like mechanical properties and suitable electrical properties. However, previously developed PEDOT:PSS inks have not been able to fully utilize the advantages of commercial 3D printing due to its long post treatment times, difficulty in high aspect ratio printing, and low conductivity. We propose a one-shot strategy for the fabrication of PEDOT:PSS ink that is able to simultaneously achieve on-demand biocompatibility (no post treatment), structural integrity during 3D printing for tall three-dimensional structures, and high conductivity for rapid-prototyping. By using ionic liquid-facilitated PEDOT:PSS colloidal stacking induced by a centrifugal protocol, a viscoplastic PEDOT:PSS-ionic liquid colloidal (PILC) ink was developed. PILC inks exhibit high-aspect ratio vertical stacking, omnidirectional printability for generating suspended architectures, high conductivity (~286 S/cm), and high-resolution printing (~50 µm). We demonstrate the on-demand and versatile applicability of PILC inks through the fabrication of 3D circuit boards, on-skin physiological signal monitoring e-tattoos, and implantable bioelectronics (opto-electrocorticography recording, low voltage sciatic nerve stimulation and recording from deeper brain layers via 3D vertical spike arrays).

Ultra-soft and highly stretchable tissue-adhesive hydrogel based multifunctional implantable sensor for monitoring of overactive bladder.

A highly stretchable and tissue-adhesive multifunctional sensor based on structurally engineered islets embedded in ultra-soft hydrogel is reported for monitoring of bladder activity in overactive bladder (OAB) induced rat and anesthetized pig. The use of hydrogel yielded a much lower sensor modulus (1 kPa) compared to that of the bladder (300 kPa), while the strong adhesiveness of the hydrogel (adhesive strength: 260.86 N/m) allowed firm attachment onto the bladder. The change in resistance of printed liquid metal particle thin-film lines under strain were used to detect bladder inflation and deflation; due to the high stretchability and reliability of the lines, surface strains of 200% could be measured repeatedly. Au electrodes coated with Platinum black were used to detect electromyography (EMG). These electrodes were placed on structurally engineered rigid islets so that no interfacial fracture occurs under high strains associated with bladder expansion. On the OAB induced rat, stronger signals (change in resistance and EMG root-mean-square) were detected near intra-bladder pressure maxima, thus showing correlation to bladder activity. Moreover, using robot-assisted laparoscopic surgery, the sensor was placed onto the bladder of an anesthetized pig. Under voiding and filling, bladder strain and EMG were once again monitored. These results confirm that our proposed sensor is a highly feasible, clinically relevant implantable device for continuous monitoring OAB for diagnosis and treatment.

Conductance stable and mechanically durable bi-layer EGaIn composite-coated stretchable fiber for 1D bioelectronics.

Deformable semi-solid liquid metal particles (LMP) have emerged as a promising substitute for rigid conductive fillers due to their excellent electrical properties and stable conductance under strain. However, achieving a compact and robust coating of LMP on fibers remains a persistent challenge, mainly due to the incompatibility of conventional coating techniques with LMP. Additionally, the limited durability and absence of initial electrical conductivity of LMP restrict their widespread application. In this study, we propose a solution process that robustly and compactly assembles mechanically durable and initially conductive LMP on fibers. Specifically, we present a shearing-based deposition of polymer-attached LMP followed by additional coating with CNT-attached LMP to create bi-layer LMP composite with exceptional durability, electrical conductivity, stretchability, and biocompatibility on various fibers. The versatility and reliability of this manufacturing strategy for 1D electronics are demonstrated through the development of sewn electrical circuits, smart clothes, stretchable biointerfaced fiber, and multifunctional fiber probes.

Photoswitchable Microgels for Dynamic Macrophage Modulation.

Dynamic manipulation of supramolecular self-assembled structures is achieved irreversibly or under non-physiological conditions, thereby limiting their biomedical, environmental, and catalysis applicability. In this study, microgels composed of azobenzene derivatives stacked via π-cation and π-π interactions are developed that are electrostatically stabilized with Arg-Gly-Asp (RGD)-bearing anionic polymers. Lateral swelling of RGD-bearing microgels occurs via cis-azobenzene formation mediated by near-infrared-light-upconverted ultraviolet light, which disrupts intermolecular interactions on the visible-light-absorbing upconversion-nanoparticle-coated materials. Real-time imaging and molecular dynamics simulations demonstrate the deswelling of RGD-bearing microgels via visible-light-mediated trans-azobenzene formation. Near-infrared light can induce in situ swelling of RGD-bearing microgels to increase RGD availability and trigger release of loaded interleukin-4, which facilitates the adhesion structure assembly linked with pro-regenerative polarization of host macrophages. In contrast, visible light can induce deswelling of RGD-bearing microgels to decrease RGD availability that suppresses macrophage adhesion that yields pro-inflammatory polarization. These microgels exhibit high stability and non-toxicity. Versatile use of ligands and protein delivery can offer cytocompatible and photoswitchable manipulability of diverse host cells.

Neuromorphic Processing of Pressure Signal Using Integrated Sensor-Synaptic Device Capable of Selective and Reversible Short- and Long-Term Plasticity Operation.

To mimic the tactile sensing properties of the human skin, signals from tactile sensors need to be processed in an efficient manner. The integration of the tactile sensor with a neuromorphic device can potentially address this issue, as the neuromorphic device has both signal processing and memory capability through which parallel and efficient processing of information is possible. In this article, an intelligent haptic perception device (IHPD) is presented that combines pressure sensing with an organic electrochemical transistor-based synaptic device into a simple device architecture. More importantly, the IHPD is capable of rapid and reversible switching between short-term plasticity (STP) and long-term plasticity (LTP) operation through which accelerated learning, processing of new information, and distinctive operation of STP and LTP are possible. Various types of pressure information such as magnitude, rate, and duration were processed utilizing STP by which error-tolerant perception was demonstrated. Meanwhile, memorization and learning of pressure through a stepwise change in a conductive state was demonstrated using LTP. These demonstrations present unique approaches to process and learn tactile information, which can potentially be utilized in various electronic skin applications in the future.

Parallel Signal Processing of a Wireless Pressure-Sensing Platform Combined with Machine-Learning-Based Cognition, Inspired by the Human Somatosensory System.

Inspired by the human somatosensory system, pressure applied to multiple pressure sensors is received in parallel and combined into a representative signal pattern, which is subsequently processed using machine learning. The pressure signals are combined using a wireless system, where each sensor is assigned a specific resonant frequency on the reflection coefficient (S11 ) spectrum, and the applied pressure changes the magnitude of the S11 pole with minimal frequency shift. This allows the differentiation and identification of the pressure applied to each sensor. The pressure sensor consists of polypyrrole-coated microstructured poly(dimethylsiloxane) placed on top of electrodes, operating as a capacitive sensor. The high dielectric constant of polypyrrole enables relatively high pressure-sensing performance. The coils are vertically stacked to enable the reader to receive the signals from all of the sensors simultaneously at a single location, analogous to the junction between neighboring primary neurons to a secondary neuron. Here, the stacking order is important to minimize the interference between the coils. Furthermore, convolutional neural network (CNN)-based machine learning is utilized to predict the applied pressure of each sensor from unforeseen S11 spectra. With increasing training, the prediction accuracy improves (with mean squared error of 0.12), analogous to humans' cognitive learning ability.

Electronic Skin: Recent Progress and Future Prospects for Skin-Attachable Devices for Health Monitoring, Robotics, and Prosthetics.

Recent progress in electronic skin or e-skin research is broadly reviewed, focusing on technologies needed in three main applications: skin-attachable electronics, robotics, and prosthetics. First, since e-skin will be exposed to prolonged stresses of various kinds and needs to be conformally adhered to irregularly shaped surfaces, materials with intrinsic stretchability and self-healing properties are of great importance. Second, tactile sensing capability such as the detection of pressure, strain, slip, force vector, and temperature are important for health monitoring in skin attachable devices, and to enable object manipulation and detection of surrounding environment for robotics and prosthetics. For skin attachable devices, chemical and electrophysiological sensing and wireless signal communication are of high significance to fully gauge the state of health of users and to ensure user comfort. For robotics and prosthetics, large-area integration on 3D surfaces in a facile and scalable manner is critical. Furthermore, new signal processing strategies using neuromorphic devices are needed to efficiently process tactile information in a parallel and low power manner. For prosthetics, neural interfacing electrodes are of high importance. These topics are discussed, focusing on progress, current challenges, and future prospects.

PVDF-Based Piezoelectric Microphone for Sound Detection Inside the Cochlea: Toward Totally Implantable Cochlear Implants.

We report the fabrication and characterization of a prototype polyvinylidene fluoride polymer-based implantable microphone for detecting sound inside gerbil and human cochleae. With the current configuration and amplification, the signal-to-noise ratios were sufficiently high for normally occurring sound pressures and frequencies (ear canal pressures >50-60 dB SPL and 0.1-10 kHz), though 10 to 20 dB poorer than for some hearing aid microphones. These results demonstrate the feasibility of the prototype devices as implantable microphones for the development of totally implantable cochlear implants. For patients, this will improve sound reception by utilizing the outer ear and will improve the use of cochlear implants.

Wafer-scale fabrication and characterization of thin-film transistors with polythiophene-sorted semiconducting carbon nanotube networks.

Semiconducting single-walled carbon nanotubes (SWCNTs) have great potential of becoming the channel material for future thin-film transistor technology. However, an effective sorting technique is needed to obtain high-quality semiconducting SWCNTs for optimal device performance. In our previous work, we reported a dispersion technique for semiconducting SWCNTs that relies on regioregular poly(3-dodecylthiophene) (rr-P3DDT) to form hybrid nanostructures. In this study, we demonstrate the scalability of those sorted CNT composite structures to form arrays of TFTs using standard lithographic techniques. The robustness of these CNT nanostructures was tested with Raman spectroscopy and atomic force microscope images. Important trends in device properties were extracted by means of electrical measurements for different CNT concentrations and channel lengths (L(c)). A statistical study provided an average mobility of 1 cm(2)/V·s and I(on)/I(off) as high as 10(6) for short channel lengths (L(c) = 1.5 µm) with 100% yield. This highlights the effectiveness of this sorting technique and its scalability for large-scale, flexible, and transparent display applications.

Selective dispersion of high purity semiconducting single-walled carbon nanotubes with regioregular poly(3-alkylthiophene)s.

Conjugated polymers, such as polyfluorene and poly(phenylene vinylene), have been used to selectively disperse semiconducting single-walled carbon nanotubes (sc-SWNTs), but these polymers have limited applications in transistors and solar cells. Regioregular poly(3-alkylthiophene)s (rr-P3ATs) are the most widely used materials for organic electronics and have been observed to wrap around SWNTs. However, no sorting of sc-SWNTs has been achieved before. Here we report the application of rr-P3ATs to sort sc-SWNTs. Through rational selection of polymers, solvent and temperature, we achieved highly selective dispersion of sc-SWNTs. Our approach enables direct film preparation after a simple centrifugation step. Using the sorted sc-SWNTs, we fabricate high-performance SWNT network transistors with observed charge-carrier mobility as high as 12 cm(2) V(-1) s(-1) and on/off ratio of >10(6). Our method offers a facile and a scalable route for separating sc-SWNTs and fabrication of electronic devices.

Synthetic PAMAM-RGD conjugates target and bind to odontoblast-like MDPC 23 cells and the predentin in tooth organ cultures.

Screening techniques now allow for the identification of small peptides that bind specifically to molecules like cells. However, despite the enthusiasm for this approach, single peptides often lack the binding affinity to target in vivo and regulate cell function. We took peptides containing the Arg-Gly Asp(RGD) motif that bind to the alpha Vbeta 3 integrin and have shown potential as therapeutics. To improve their binding affinity, we synthesized polyamidoamine (PAMAM) dendrimer-RGD conjugates that that contain 12-13 copies of the peptide. When cultured with human dermal microvessel endothelial cells (HDMEC), human vascular endothelial cells (HUVEC), or odontoblast-like MDPC-23 cells, the PAMAM dendrimer conjugate targets this receptor in a manner that is both time- and dose-dependent. Finally, this conjugate selectively targets RGD binding sites in the predentin of human tooth organ cultures. Taken together, these studies provide proof of principle that synthetic PAMAM-RGD conjugates could prove useful as carriers for the tissue-specific delivery of integrin-targeted therapeutics or imaging agents and could be used to engineer tissue regeneration.