Browsing by Subject "Printed electronics"

In the field of electronic materials, metal nanowires have been extensively studied for both their syntheses and their properties in electronic composites and devices. This dissertation addresses challenges in the field of electronic materials development with the use of copper nanowires synthesized in gram-scale syntheses, as well as provides analysis of devices and composites that could only be feasibly manufactured thanks to the large-scale syntheses.

In the field of printed electronics, there has been research into the development of fully printed memories. One of the challenges has been developing a memory that has switching characteristics that are on par with existing commercial memories, such as Flash memory. This can be achieved with a composite of Cu-SiO2 nanowires dispersed in ethylcellulose, which acts as a resistive switch when between printed Cu and Au electrodes. A 16-cell crossbar array of these memristors was printed with an aerosol jet. The memristors exhibited moderate operating voltages (~3 V), no degradation over 104 switching cycles, write speeds of 3 µs, and extrapolated retention times of 10 years. The low operating voltage enabled the programming of a fully printed 4-bit memristor array with an Arduino. The excellent performance of these fully printed memristors could help enable the creation of fully printed RFID tags and sensors with integrated data storage. Thanks to the large-scale synthesis of copper nanowires, this can allow for the expanded production of high-quality, fully printed memories.

Materials that retain a high conductivity under strain are essential for wearable electronics. I describe a new conductive, stretchable composite consisting of a Cu-Ag core-shell nanowire felt infiltrated with a silicone elastomer. This composite exhibits a retention of conductivity under strain that is superior to any composite with a conductivity greater than 1000 S cm-1. This work also shows how the mechanical properties, conductivity, and deformation mechanisms of the composite changes as a function of the stiffness of the silicone matrix. The retention of conductivity under strain was found to decrease as the Young’s modulus of the matrix increased. This was attributed to void formation as a result of debonding between the nanowire felt and the elastomer. The nanowire composite was also patterned to create serpentine circuits with a stretchability of 300%. Composites of this scale and density could only be feasibly manufactured thanks to large-scale syntheses of copper nanowires and the silver coating of copper nanowires. With the advances made in the quality of stretchable conductive composites, alternate methods were employed as to manufacture new composites and structures, such as the cofiltration of nanowires and waterborne rubber to accelerate production, or the manufacturing of Cu-Ag nanowire aerogels with density tunable via the aspect ratio of the nanowires.

As the cost of medical care increases, people are relying increasingly on internet diagnosis and community care rather than the expertise of medical professionals. Technological and medical advances have facilitated a partial answer through the increase in handheld sensing apparatuses. Yet even with these developments, significant further advancements are required to further drive down fabrication requirements (both in terms of cost and environmental impact) and facilitate fully-integrated and easy to use sensors. Printing electronics could be a powerful tool to accomplish this as printing allows for low-cost fabrication of high-area electronics. The vast majority of printed electronics reports focus on utilization of already developed commercial inks to create devices with new functionalities. This significantly limits development because current inks both necessitate damaging post processing—which precludes the use of delicate substrates, making skin-integration impossible—and many inks require bespoke printing processes, which increases fabrication complexity and thus cost. Further, with the proliferation of single-use medical testing, consideration must be made towards environmental compatibility. Therefore, innovations in electronic ink formulation and printing geared towards addressing the post-processing and environmental impact concerns are needed to enable continued progress towards printed POC sensors. The work contained in this dissertation centers around the development of inks intended to advance electronic biosensing applications. Focus is on using aerosol jet printing to enable the printing of nanomaterials and utilizes the unique properties of these nanomaterials—such as functionality immediately after printing, recyclability, and compatibility with deposition directly on biological surfaces (i.e., human skin)—to develop technologies intended to democratize healthcare. Notably, low temperature printable silver nanowire (AgNW) inks for the creation of biologically integrated electronics are demonstrated. Electrically conductive inks are created that are capable of achieving high conductivities when directly deposited onto living tissue at temperatures compatible with life (20 °C). The conductive lines yielded high resistance to degradation from bending strain, with a mere 8% decrease in conductivity when the plastic film on which they were printed was folded in half. As a demonstration, the AgNW ink was printed onto a human finger and used to illuminate a small light that remained illuminated even when the finger was bent. These results pave the way towards patient-specific medical diagnostics that are comfortable to wear, easy to use, and designed towards the needs of each individual patient. Next, a printing method to deposit biological sensing proteins for biomedical assays is investigated. Traditional techniques require extended time and the use of large quantities of immensely expensive proteins to make biosensors. Herein, a decade-old belief that aerosol jet printing is incompatible with the deposition of proteins is overturned, and, in doing so, highly sensitive biosensors for carcinoembryonic antigen (CEA) that compare favorably the mainstay fabrication technique that is known to impart no damage to the printed biological inks is demonstrated. Finally, the co-printing of a bio-recognition element with the previously mentioned electrically conductive AgNW ink demonstrate the potential for the future investigation of a fully aerosol-jet printed electronic biosensor. To address the environmental waste accumulation concern that plagues the advancement of ubiquitous patient-guided sensing, inks that facilitate the creation of fully-printed, all-carbon recyclable electronics (ACRE) are investigated. The combination of nanocrystalline cellulose, graphene and semiconducting carbon nanotubes enable the first fully recyclable transistor device. The ACRE transistors maintain high stability for over 10 months, display among the best performance of any printed transistor (Ion/Ioff: 104 and Ion 65 µA µm-1) and can be entirely deconstructed for recapture and reuse of the constituent CNT and graphene inks with near 100% nanomaterial retention and the biodegradation of the cellulose-based components. ACRE-based lactate sensors are used as an illustration of utility to show the versatility of the platform. Finally, as a culminating demonstration, a fully-printed chip for the handheld measurement of blood clot time (prothrombin time) was developed. Printing the entirety of the device allows for the creation of a low-cost chip for the simple, fast, and robust measurement of human blood clot times. In addition, a custom-designed, handheld control system with a 3D-printed case was developed to create a fully integrated point-of-care measurement platform towards simplifying medicine dosing strategies. The work described herein marks a significant leap in the development of printed inks to enable custom biological sensing applications. Once fully realized, these applications will mark a watershed, ushering in an era of individualized medicine with ubiquitous sensing to actively track disease progression in real-time. We are at the dawn of a new era in medicine that focuses more on prevention and control as opposed to reaction. One future direction for this work is promoting directly printed and reusable on-skin theragnostics for bespoke patient care such as the delivery and monitoring of pain medication that allows for better oversite over use and misuse.

As the Internet of Things (IoT) continues to expand, there is increasing demand for custom low-cost sensors, displays, and communication devices that can grow and diversify the electronics ecosystem. The benefits to society of a vibrant, ubiquitous IoT include improved safety, health, and productivity as larger and more relevant datasets are able to be generated for fueling game-changing artificial intelligence and machine learning models. Printed carbon nanotube thin-film transistors (CNT-TFTs) have emerged as preeminent devices for enabling potentially transformative capabilities from, and widespread use of, IoT electronics. Still, despite intensive research over the past 15 years, there has yet to be the development of a streamlined, direct-write, in-place printing process, similar to today’s widely used inkjet or 3D printing technologies, where the substrate never leaves the printing stage and requires little to no post-processing. The development of such a process for producing CNT-TFTs could lead to the emergence of print-on-demand electronics, where direct-write printers are capable of printing distinct IoT sensing devices or even full IoT systems with little to no user intervention.

The work contained in this dissertation describes discoveries and innovations for streamlining and optimizing direct-write printed electronics using in-line or in-place methods, with primary focus on an in-place printing process for producing CNT-TFTs at relatively low temperature. The key enabling aspect of the in-place printing of CNT-TFTs was the development of aerosol jet-printable low-temperature conductive and dielectric inks that are functional immediately after printing. Additionally, the printed semiconducting CNT films required modified rinsing procedures for in-line processing, which proved to enhance performance. Notably, the resulting CNT-TFTs exhibited promising performance metrics with on/off-current ratios exceeding 103 and mobilities up to 11 cm2V-1s-1, while also operating under mechanical strain or after long-term bias stress, despite being printed with a maximum process temperature of only 80 °C. While optimizing these devices, various contact morphologies and configurations were investigated, where it was found that there was less variability in performance between sets of top-contacted devices, compared to bottom-contacts. Additionally, it was discovered that there are processing and performance trade-offs associated with various contact morphologies, with silver nanowires holding most value for in-place printing.

Although primary focus is given to aerosol jet-printed, CNT-based devices, this work also outlines another rapid, and potentially in-line, process for improving IoT-relevant electronics printed from a widely used direct-write method: fused filament fabrication. Here, using a high intensity flash lamp, the conductance of thermoplastic filaments are enhanced by up to two orders of magnitude. It was found that high-intensity light vaporizes the topmost layer of thermoplastic on metal-composite filaments, leaving behind a metallized surface layer in a technique referred to as flash ablation metallization (FAM). FAM was then used to enhance the performance of 3D printed circuit boards, demonstrating use in an immediately relevant application.

Overall, the development of in-place printed CNT-TFTs and the FAM process establish practical and scientific foundations for continued progress toward print-on-demand electronics. These foundations include: the development of low-temperature inks, rapid and in-line compatible process methods, and investigations of the impacts of various materials, device configurations, or process steps on electronic performance. Altogether, these developments have the potential to lower the time, costs, and overhead associated with printed electronics, moving the field closer to a point that is more accessible to industrialists, academics, and hobbyists alike.

With the advent of the internet-of-things (IoT) and a more connected digital ecosystem, new electronic sensors and systems are needed. Printing has been identified as a means of fabricating low-cost electronics on non-rigid, large-area substrates. Printed electronics have been demonstrated to have the required electrical and mechanical properties to facilitate new and unique flexible electronic sensors for the IoT. One printable material that has demonstrated significant promise, specifically when compared to more traditional printed semiconductors, is solution-processed carbon nanotubes (CNTs). While some work has been done to facilitate the fabrication of CNT thin-film transistors (TFTs), little work has been done to assess the viability and potential of CNT-TFTs and other CNT thin films for real-world sensing applications.

The work contained in this dissertation describes the use of aerosol jet printing to fabricate CNT-TFTs, and the resulting study of their capability for various sensing applications. Aerosol jet printing allows for printing all the materials necessary for a fully-functional CNT-TFT, including the semiconducting thin film, conducting contacts and gate, and insulating gate dielectric. Using this system, flexible and fully printed CNT-TFTs were developed and characterized. Fully printed transistors were fabricated with field-effect mobilities as a high as 16 cm2/(Vs). The transistors were also resilient to substantial bending/strain, showing no measurable performance degradation after 1000 bending cycles at a radius of curvature of 1 mm.

The printed CNT-TFTs were evaluated for several sensing applications, including environmental pressure sensing and point-of-care biological sensing. The biological sensors, which were electronically transduced immunoassays, consisted of an antifouling polymer brush layer to enhance the CNT-TFT sensitivity and printed antibodies for detection of target analytes. Unparalleled sensitivity in unfiltered biological milieus was realized with these printed biosensors, detecting protein concentrations as low as 10 pg/ml in whole blood. In addition to demonstrating an electronically transduced TFT-based biosensor, work was done to develop a stable platform with high yield that will provide the means for a deeper understanding of the biosensing mechanisms of transistor-based sensors. As part of this biosensor platform development, novel solution-gated CNT-TFTs were demonstrated, with stable operation in ionic solutions for periods as long as 5 hours.

Another important electronic sensing technique is capacitive-based sensing. Using aerosol jet printed carbon nanotubes, a capacitive sensor has been developed and demonstrated for measuring insulating material thickness. The sensors rely on the fringing field between two adjacent electrodes interacting with the material out-of-plane, and that interaction being perturbed differently based on the thickness of the overlaid material. This sensor was also demonstrated in a one-dimensional array, which can be used to map tire tread thickness from the outside of the tire.

Overall, this dissertation explores the use of printed carbon nanotubes for diverse sensing applications. While this work provides real-world demonstrations that have potential impact for the IoT, there are also substantial scientific advancements made. Namely, insight into biosensing mechanisms, operation of solution-gated nanomaterial-based transistors, and demonstration of porosity and thickness effects on printed capacitive sensor electrodes.