Printed Platinum Nanoparticle Thin-Film Structures for Use in Biology and Catalysis: Synthesis, Printing, and Application Demonstration.

This work describes the formulation of a stable platinum nanoparticle-based ink for drop-on-demand inkjet printing and fabrication of metallic platinum thin films. A highly conductive functional nanoink was formulated based on dodecanethiol platinum nanoparticles (3-5 nm) dispersed in a toluene-terpineol mixture with a loading of 15 wt %, compatible with inkjet printing. The reduced sintering temperatures (200 °C) make them interesting for integration in devices using flexible substrates and substrates that cannot tolerate high-temperature exposures. A resistive platinum heater was successfully printed as a demonstrator for integration of the platinum ink. The platinum nanoink developed herein will be, therefore, attractive for a range of applications in biology, chemistry, and printed electronics.

In Situ Observations of Nanofibril Nucleation and Growth during the Electrochemical Polymerization of Poly(3,4-ethylenedioxythiophene) Using Liquid-Phase Transmission Electron Microscopy.

The electrochemical deposition of poly(3,4-ethylenedioxythiophene) (PEDOT) has been carried out previously in the presence of a variety of counterions. Previous studies have shown that elongated nanofibrillar structures of PEDOT would form reproducibly when certain counterions such as poly(acrylic acid) (PAA) were added to the reaction mixture. However, details of the nanofibril nucleation and growth stages were not yet clear. Here, we describe the structural evolution of PEDOT nanofibrils using liquid-phase transmission electron microscopy (LPTEM). We measured the growth velocities of nanofibrils in different directions at various stages of the process and their intensity profiles, and we have estimated the number of EDOT monomers involved. We observed that fibrils initially grew anisotropically in a direction nominally perpendicular to the local edge of the electrodes, with rates that were faster along their lengths as compared those along to their widths and thicknesses. These real-time observations have helped us elucidate the nucleation and growth of PEDOT nanofibrils during electrochemical deposition.

Printed flexible and transparent electronics: enhancing low-temperature processed metal oxides with 0D and 1D nanomaterials.

Metal oxides have broad multifunctionality and important applications to energy, sensing, and information display. Printed electronics have recently adopted metal oxides to push the limits of performance and stability for flexible thin film systems. However, a grand challenge in this field is to achieve these properties while balancing the thermal budget, which critically determines the applicability, flexibility, and cost of these systems. This paper presents a focused review of printed metal oxide electronics, highlighting our recent work developing high-performance, printed transistors processed at low temperatures via aqueous precursor chemistries, nanomaterial hybrid inks, and ultraviolet annealing. These results reveal the potential for printing uniquely high-performance active devices (electronic mobility >10 cm2 V-1 s-1) but also illustrates the utility of nanocomposites that integrate nanomaterials within a metal oxide matrix for improving device performance.

Principles of Moisturizer Product Design

Moisturizers provide significant benefit in dermatology ­ as adjuvant therapy for many clinical conditions, as a key player in anti-aging regimens, and as a core component in maintaining healthy skin barrier function. Although they have been a mainstay for decades, lotions and creams are no longer formulated with a one-size-fits-all approach, where thickness was the primary cue for efficacy. In fact, moisturizer design today has become an art as well as a science. Product efficacy, aesthetics, and packaging are all engineered in a variety of ways, to create an expansive market of products that meet many consumer needs. The addition of specific types of functional ingredients can make a noteworthy difference as well. This article will explore the myriad approaches for moisturizer development and debunk some of the long-standing myths that have pervaded the marketplace. J Drugs Dermatol. 2019;18(1 Suppl):s89-95

Scalable, High-Performance Printed InO x Transistors Enabled by Ultraviolet-Annealed Printed High- k AlO x Gate Dielectrics.

Inorganic transparent metal oxides represent one of the highest performing material systems for thin-film flexible electronics. Integrating these materials with low-temperature processing and printing technologies could fuel the next generation of ubiquitous transparent devices. In this work, we investigate the integration of UV-annealing with inkjet printing, demonstrating how UV-annealing of high- k AlO x dielectrics facilitates the fabrication of high-performance InO x transistors at low processing temperatures and improves bias-stress stability of devices with all-printed dielectrics, semiconductors, and source/drain electrodes. First, the influence of UV-annealing on printed metal-insulator-metal capacitors is explored, illustrating the effects of UV-annealing on the electrical, chemical, and morphological properties of the printed gate dielectrics. Utilizing these dielectrics, printed InO x transistors were fabricated which achieved exceptional performance at low process temperatures (<250 °C), with linear mobility µlin ≈ 12 ± 1.6 cm2/V s, subthreshold slope <150 mV/dec, Ion/ Ioff > 107, and minimal hysteresis (<50 mV). Importantly, detailed characterization of these UV-annealed printed devices reveals enhanced operational stability, with reduced threshold voltage ( Vt) shifts and more stable on-current. This work highlights a unique, synergistic interaction between low-temperature-processed high- k dielectrics and printed metal oxide semiconductors.

In situ electrochemical polymerization of poly(3,4-ethylenedioxythiophene) (PEDOT) for peripheral nerve interfaces.

The goal of this study was to perform in situ electrochemical polymerization of poly(3,4-ethylenedioxythiophene) (PEDOT) in peripheral nerves to create a soft, precisely located injectable conductive polymer electrode for bi-directional communication. Intraneural PEDOT polymerization was performed to target both outer and inner fascicles via custom fabricated 3D printed cuff electrodes and monomer injection strategies using a combination electrode-cannula system. Electrochemistry, histology, and laser light sheet microscopy revealed the presence of PEDOT at specified locations inside of peripheral nerve. This work demonstrates the potential for using in situ PEDOT electrodeposition as an injectable electrode for recording and stimulation of peripheral nerves.

Printed unmanned aerial vehicles using paper-based electroactive polymer actuators and organic ion gel transistors.

We combined lightweight and mechanically flexible printed transistors and actuators with a paper unmanned aerial vehicle (UAV) glider prototype to demonstrate electrically controlled glide path modification in a lightweight, disposable UAV system. The integration of lightweight and mechanically flexible electronics that is offered by printed electronics is uniquely attractive in this regard because it enables flight control in an inexpensive, disposable, and easily integrated system. Here, we demonstrate electroactive polymer (EAP) actuators that are directly printed into paper that act as steering elements for low cost, lightweight paper UAVs. We drive these actuators by using ion gel-gated organic thin film transistors (OTFTs) that are ideally suited as drive transistors for these actuators in terms of drive current and frequency requirements. By using a printing-based fabrication process on a paper glider, we are able to deliver an attractive path to the realization of inexpensive UAVs for ubiquitous sensing and monitoring flight applications.

Scalability of carbon-nanotube-based thin film transistors for flexible electronic devices manufactured using an all roll-to-roll gravure printing system.

To demonstrate that roll-to-roll (R2R) gravure printing is a suitable advanced manufacturing method for flexible thin film transistor (TFT)-based electronic circuits, three different nanomaterial-based inks (silver nanoparticles, BaTiO3 nanoparticles and single-walled carbon nanotubes (SWNTs)) were selected and optimized to enable the realization of fully printed SWNT-based TFTs (SWNT-TFTs) on 150-m-long rolls of 0.25-m-wide poly(ethylene terephthalate) (PET). SWNT-TFTs with 5 different channel lengths, namely, 30, 80, 130, 180, and 230 µm, were fabricated using a printing speed of 8 m/min. These SWNT-TFTs were characterized, and the obtained electrical parameters were related to major mechanical factors such as web tension, registration accuracy, impression roll pressure and printing speed to determine whether these mechanical factors were the sources of the observed device-to-device variations. By utilizing the electrical parameters from the SWNT-TFTs, a Monte Carlo simulation for a 1-bit adder circuit, as a reference, was conducted to demonstrate that functional circuits with reasonable complexity can indeed be manufactured using R2R gravure printing. The simulation results suggest that circuits with complexity, similar to the full adder circuit, can be printed with a 76% circuit yield if threshold voltage (Vth) variations of less than 30% can be maintained.

Gravure-Printed Sol-Gels on Flexible Glass: A Scalable Route to Additively Patterned Transparent Conductors.

Gravure printing is an attractive technique for patterning high-resolution features (<5 µm) at high speeds (>1 m/s), but its electronic applications have largely been limited to depositing nanoparticle inks and polymer solutions on plastic. Here, we extend the scope of gravure to a new class of materials and on to new substrates by developing viscous sol-gel precursors for printing fine lines and films of leading transparent conducting oxides (TCOs) on flexible glass. We explore two strategies for controlling sol-gel rheology: tuning the precursor concentration and tuning the content of viscous stabilizing agents. The sol-gel chemistries studied yield printable inks with viscosities of 20-160 cP. The morphology of printed lines of antimony-doped tin oxide (ATO) and tin-doped indium oxide (ITO) is studied as a function of ink formulation for lines as narrow as 35 µm, showing that concentrated inks form thicker lines with smoother edge morphologies. The electrical and optical properties of printed TCOs are characterized as a function of ink formulation and printed film thickness. XRD studies were also performed to understand the dependence of electrical performance on ink composition. Printed ITO lines and films achieve sheet resistance (Rs) as low as 200 and 100 Ω/□, respectively (ρ≈2×10(-3) Ω-cm) for single layers. Similarly, ATO lines and films have Rs as low as 700 and 400 Ω/□ with ρ≈7×10(-3) Ω-cm. High visible range transparency is observed for ITO (86-88%) and ATO (86-89%). Finally, the influence of moderate bending stress on ATO films is investigated, showing the potential for this work to scale to roll-to-roll (R2R) systems.

Tailoring indium oxide nanocrystal synthesis conditions for air-stable high-performance solution-processed thin-film transistors.

Semiconducting metal oxides (ZnO, SnO2, In2O3, and combinations thereof) are a uniquely interesting family of materials because of their high carrier mobilities in the amorphous and generally disordered states, and solution-processed routes to these materials are of particular interest to the printed electronics community. Colloidal nanocrystal routes to these materials are particularly interesting, because nanocrystals may be formulated with tunable surface properties into stable inks, and printed to form devices in an additive manner. We report our investigation of an In2O3 nanocrystal synthesis for high-performance solution-deposited semiconductor layers for thin-film transistors (TFTs). We studied the effects of various synthesis parameters on the nanocrystals themselves, and how those changes ultimately impacted the performance of TFTs. Using a sintered film of solution-deposited In2O3 nanocrystals as the TFT channel material, we fabricated devices that exhibit field effect mobility of 10 cm(2)/(V s) and an on/off current ratio greater than 1 × 10(6). These results outperform previous air-stable nanocrystal TFTs, and demonstrate the suitability of colloidal nanocrystal inks for high-performance printed electronics.

High-performance inkjet-printed four-terminal microelectromechanical relays and inverters.

We report the first demonstration of inkjet-printed 4-terminal microelectromechanical (MEM) relays and inverters with hyper-abrupt switching that exhibit excellent electrical and mechanical characteristics. This first implementation of a printed 4-terminal device is critically important, since it allows for the realization of full complementary logic functions. The floated fourth terminal (body electrode), which allows the gate switching voltage to be adjusted, is bonded to movable channel beams via a printed epoxy layer in a planar structure, which can move downward together via the electrostatic force between the gate electrodes and body such that the channel can also actuate downward and touch the drain electrode. Because the body, channel, and drain electrodes are completely electrically separated, no detectable leakage or electrical interference between the electrodes is observed. The printed MEM relay exhibited an on-state resistance of only 3.48 Ω, immeasurable off-state leakage, subthreshold swing <1 mV/dec, and a stable operation over 10(4) cycles with a switching delay of 47 µs, and the relay inverter exhibits abrupt transitions between on/off states. The operation of the printed 4-terminal MEM relay was also verified against the results of a 3-dimensional (3D) finite element simulation.

Impedance sensing device enables early detection of pressure ulcers in vivo.

When pressure is applied to a localized area of the body for an extended time, the resulting loss of blood flow and subsequent reperfusion to the tissue causes cell death and a pressure ulcer develops. Preventing pressure ulcers is challenging because the combination of pressure and time that results in tissue damage varies widely between patients, and the underlying damage is often severe by the time a surface wound becomes visible. Currently, no method exists to detect early tissue damage and enable intervention. Here we demonstrate a flexible, electronic device that non-invasively maps pressure-induced tissue damage, even when such damage cannot be visually observed. Using impedance spectroscopy across flexible electrode arrays in vivo on a rat model, we find that impedance is robustly correlated with tissue health across multiple animals and wound types. Our results demonstrate the feasibility of an automated, non-invasive 'smart bandage' for early detection of pressure ulcers.

Impedance sensing device for monitoring ulcer healing in human patients.

Chronic skin wounds affect millions of people each year and take billions of dollars to treat. Ulcers are a type of chronic skin wound that can be especially painful for patients and are tricky to treat because current monitoring solutions are subjective. We have developed an impedance sensing tool to objectively monitor the progression of healing in ulcers, and have begun a clinical trial to evaluate the safety and feasibility of our device to map damaged regions of skin. Impedance data has been collected on five patients with ulcers, and impedance was found to correlate with tissue health. A damage threshold was applied to effectively identify certain regions of skin as "damaged tissue".

A stencil printed, high energy density silver oxide battery using a novel photopolymerizable poly(acrylic acid) separator.

A novel photopolymerized poly(acrylic acid) separator is demonstrated in a printed, high-energy-density silver oxide battery. The printed battery demonstrates a high capacity of 5.4 mA h cm(-2) at a discharge current density of 2.75 mA cm(-2) (C/2 rate) while delivering good mechanical flexibility and robustness.

Cell filling in gravure printing for printed electronics.

Highly scaled direct gravure is a promising printing technique for printed electronics due to its large throughput, high resolution, and simplicity. Gravure can print features in the single micron range at printing speeds of ∼1 m/s by using an optimized cell geometry and optimized printing conditions. The filling of the cells on the gravure cylinder is a critical process, since the amount of ink in the cells strongly impacts printed feature size and quality. Therefore, an understanding of cell filling is crucial to make highly scaled gravure printed electronics viable. In this work we report a novel experimental setup to investigate the filling process in real time, coupled with numerical simulations to gain insight into the experimental observations. By varying viscosity and filling speed, we ensure that the dimensionless capillary number is a good indicator of filling regime in real gravure printing. In addition, we also examine the effect of cell size on filling as this is important for increasing printing resolution. In the light of experimental and simulation results, we are able to rationalize the dominant failure in the filling process, i.e., air entrapment, which is caused by contact line pinning and interface deformation over the cell opening.

Systematic design of jettable nanoparticle-based inkjet inks: rheology, acoustics, and jettability.

Drop-on-demand inkjet printing of functional inks has received a great deal of attention for realizing printed electronics, rapidly prototyped structures, and large-area systems. Although this method of printing promises high processing speeds and minimal substrate contamination, the performance of this process is often limited by the rheological parameters of the ink itself. Effective ink design must address a myriad of issues, including suppression of the coffee-ring effect, proper drop pinning on the substrate, long-term ink reliability, and, most importantly, stable droplet formation, or jettability. In this work, by simultaneously considering optimal jetting conditions and ink rheology, we develop and experimentally validate a jettability window within the capillary number-Weber number space. Furthermore, we demonstrate the exploitation of this window to adjust nanoparticle-based ink rheology predictively to realize a jettable ink. Finally, we investigate the influence of mass loading on jettability to establish additional practical limitations on nanoparticle ink design.

Roll-to-roll gravure with nanomaterials for printing smart packaging.

Roll-to-roll (R2R) gravure is considered one of the highest throughput tools for manufacturing inexpensive and flexible ubiquitous IT devices called "smart packaging" in which NFC (near-field communication) transponder, sensors, ADC (analog-to-digital converter), simple processor and signage are all integrated on paper or plastic foils. In this review, we show R2R gravure can be employed to print smart packaging, starting from printing simple electrodes, dielectrics, capacitors, diodes and thin film transistors with appropriate nanomaterial-based inks on plastic foils.

Chronic, wireless recordings of large-scale brain activity in freely moving rhesus monkeys.

Advances in techniques for recording large-scale brain activity contribute to both the elucidation of neurophysiological principles and the development of brain-machine interfaces (BMIs). Here we describe a neurophysiological paradigm for performing tethered and wireless large-scale recordings based on movable volumetric three-dimensional (3D) multielectrode implants. This approach allowed us to isolate up to 1,800 neurons (units) per animal and simultaneously record the extracellular activity of close to 500 cortical neurons, distributed across multiple cortical areas, in freely behaving rhesus monkeys. The method is expandable, in principle, to thousands of simultaneously recorded channels. It also allows increased recording longevity (5 consecutive years) and recording of a broad range of behaviors, such as social interactions, and BMI paradigms in freely moving primates. We propose that wireless large-scale recordings could have a profound impact on basic primate neurophysiology research while providing a framework for the development and testing of clinically relevant neuroprostheses.

Lubrication-related residue as a fundamental process scaling limit to gravure printed electronics.

In gravure printing, excess ink is removed from a patterned plate or roll by wiping with a doctor blade, leaving a thin lubrication film in the nonpatterned area. Reduction of this lubrication film is critical for gravure printing of electronics, since the resulting residue can lower device performance or even catastrophically impact circuit yield. We report on experiments and quantitative analysis of lubrication films in a highly scaled gravure printing process. We investigate the effects of ink viscosity, wiping speed, loading force, blade stiffness and blade angle on the lubrication film, and further, use the resulting data to investigate the relevant lubrication regimes associated with wiping during gravure printing. Based on this analysis, we are able to posit the lubrication regime associated with wiping during gravure printing, provide insight into the ultimate limits of residue reduction, and, furthermore, are able to provide process guidelines and design rules to achieve these limits.