Flexible electronics have demonstrated potential in a wide range of applications including wearable sensors, photovoltaics, medical devices and more, due to their properties of extreme adaptability while also being lightweight and highly robust. The main challenge standing in the way of progress in this field is the difficulty of large-scale manufacturing of these flexible electronics compared to their rigid counterparts. Microcontact printing is a form of soft lithography in which an elastomeric stamp is used to transfer sub-micron scale surface patterns onto a flexible substrate via ink monolayers. The integration of microcontact printing into a roll-to-roll (R2R) system will enable continuous printing of flexible electronics and scale it up for massive manufacturing. The proposed thesis outlines a novel mechanical design for a microcontact printer which utilizes flexural motion stages with integrated position and force sensors to control the print process on a R2R system. The printhead is designed to fit the available space on the pre-installed UMass Amherst Intelligent Sensing Laboratory test table and breadboard. The R2R system includes motorized rollers for winding/unwinding the PET (polyethylene terephthalate) web substrate, and idler rollers for guiding a web through the print system. As the central element to this design, two matching plate flexures are designed on the two ends of the printer roller to control the tilting and positioning of the print roller. Flexure mechanisms rely on bending and torsion of flexible elements: this allows them to achieve much higher precision in positioning compared to conventional mechanisms which rely on surface interaction between multiple moving parts. The print resolution target for this design is 500 nm (linewidth), based on current state-of-the-art designs [1, 2]. In the initial version of the printhead design, a total of 33 parts are custom fabricated for assembly and installation in the R2R system lab setup. These include everything from the components of the print roller, specially adapted air-bearing mounts, support structures, and connectors. The design and 4 fabrication process for every component is outlined here along with the functionality, as every component was designed with the system objectives and constraints in mind. Using SolidWorks simulation, FEA (finite element analysis) is performed for every part of the assembly that is subjected to stress in the real system, so that predictions can be made about the displacement of the motion stages and the frequency of vibration. These predictions are evaluated by comparation with the experimental results from tests conducted on the real system hardware and used to assess the quality of the fabricated assembly. The work performed in this thesis enables advancements in the assembly of an updated, optimized R2R system and has led to an experimentally functioning lab setup that is ripe for further improvements. Completion and calibration of this augmented R2R system will, in future, enable UMass Amherst in-house production of large-area flexible electronics which may be used in a wide range of applications, including medical sensors, solar cells, displays, and more. In addition to microcontact printing, this R2R system may also be applied to nanoimprint lithography, another contact-based print method, or integrated with inkjet printing, a non-contact method.

<p>Paper-based flexible devices represent a new frontier in electronics technology. The research has focused on the fabrication of the lightweight, and flexible paper-based lithium ion batteries. A lithium ion battery relies on the interplay of multiple components. These components themselves, as well as the processes used to create them, need to be adjusted and modified in order to achieve a fully flexible lithium ion battery. These components include the electrode current collector, active material, and electrolyte. By modifying these components to be fully flexible and resistant to damages caused by deformation, a fully flexible battery can be achieved.</p> <p> </p> <p>Herein, the paper-based platform utilized is key to provide flexibility for the battery components. The goal of this work not only focused on the creation of a paper-based flexible battery to be used as an integrable energy storage system for flexible devices, but also on developing methodologies and processes that can advance the emerging area of paper-based electronics, where different functional units must be fabricated within a single paper substrate. The key to make effective paper-based batteries, is to achieve a highly conductive paper structure as the base. In this work, conductive nanomaterials including carbon nanotubes (CNT) and graphene were used to fabricate conductive paper, where wood microfibers were coated with layers of these nanomaterials via layer-by-layer nanoassembly. These fibers were then combined into paper sheets. The resulting paper offers a conductive and porous base for electronic devices that utilized only small quantities of CNT or reduced graphene oxide (rGO) to provide length resistances of 468 Ω/cm and 74.6 Ω/cm, respectively for each fabricated conductive paper. </p> <p> </p> <p>Flexible lithium ion batteries were then made by using CNT paper-based electrodes and a solid polymer gel electrolyte. The electrodes were made by deposition of lithium active materials over the conductive paper and where shown to be flexible, durable, and light weight. With respect to the electrolyte, a new type of gel electrolyte based on PVDF-HFP was fabricated to overcome problems related to the use of liquid electrolytes in flexible batteries. This gel, which provides a high electrolyte uptake (450% by weight), was made by infusing both liquid and ceramic electrolytes inside a polymer gel structure and demonstrated conductivity up to 10^-4 S/cm. The paper-based battery developed with these new materials has a comparable capacity to commercial batteries and represents a flexible and light weight alternative. The use of ultra-high capacity lithium compounds as cathode materials, such as vanadium pentoxide (with theoretical capacities of 440 mAh/g) in conjunction with rGO-paper as a stand-alone electrode (with a reversible capacity 546 mAh/g) were also explored and results will be discussed. </p> <p> </p> <p>This research has led to the development of a novel method of making a fully flexible lithium ion batteries, using paper-based current collectors, leak proof polymer gel electrolytes and ultra-high capacity lithium ion active materials. Thus, flexible high conductive paper-based current collectors, polymer-gel electrolytes, vanadium based ultra-high capacity cathode electrodes, and graphene-based stand-alone paper-based anodes have been developed and tested.</p> <p> </p>

The solar cells market has an annual growth of more than 30 percent over the past 15 years. At the same time, the cost of the solar modules diminished to meet both of the rapid global demand and the technological improvements. In particular for the crystalline silicon solar cells, the workhorse of this technology. The objective of this doctoral thesis is enhancing the efficiency of c-Si solar cells while exploring the cost reduction via innovative techniques. Contact metallization and ultra-flexible wafer based c-Si solar cells are the main areas under investigation. First, Silicon-based solar cells typically utilize screen printed Silver (Ag) metal contacts which affect the optimal electrical performance. To date, metal silicide-based ohmic contacts are occasionally used for the front contact grid lines. In this work, investigation of the microstructure and the electrical characteristics of nickel monosilicide (NiSi) ohmic contacts on the rear side of c-Si solar cells has been carried out. Significant enhancement in the fill factor leading to increasing the total power conversion efficiency is observed. Second, advanced classes of modern application require a new generation of versatile solar cells showcasing extreme mechanical resilience. However, silicon is a brittle material with a fracture strains <1%. Highly flexible Si-based solar cells are available in the form thin films which seem to be disadvantageous over thick Si solar cells due to the reduction of the optical absorption with less active Si material. Here, a complementary metal oxide semiconductor (CMOS) technology based integration strategy is designed where corrugation architecture to enable an ultra-flexible solar cell module from bulk mono-crystalline silicon solar wafer with 17% efficiency. This periodic corrugated array benefits from an interchangeable solar cell segmentation scheme which preserves the active silicon thickness and achieves flexibility via interdigitated back contacts. These cells can reversibly withstand high mechanical stress as the screen-printed metals have fracture strain >15%. Furthermore, the integration of the cells is demonstrated on curved surfaces for a fully functional system. Finally, the developed flexing approach is used to fabricate three-dimensional dome-shaped cells to reduce the optical coupling losses without the use of the expensive solar tracking/tilting systems.

Electronic devices today are an integral part of human life thanks to state-of-the- art complementary metal oxide semiconductor (CMOS) technology. The progress in this area can be attributed to miniaturization driven by Moore’s Law. Further advancements in electronics are under threat from physical limits in dimensional scaling and hence new roadmaps for alternative materials and technologies are chased. Furthermore, the current era of Internet of things (IoT) and Internet of everything (IoE) has broaden the horizon to a plethora of unprecedented applications. The most prominent emerging fields are flexible and stretchable electronics. There has been significant progress in developments of flexible sensors, transistors, and alternative materials, etc. Nonetheless, there remains the unaddressed challenges of matching performance of the status-quo, packaging, interconnects, and lack of pragmatic integration schemes to readily complement existing state-of-the-art technology. In this thesis, a pragmatic heterogeneous integration strategy is presented to obtain high-performance 3D electronic systems using existing CMOS based integrated circuit (IC). Critical challenges addressed during the process are: reliable flexible interconnects, maximum area efficiency, soft-polymeric packaging, and heterogeneous integration compatible with current CMOS technology. First, a modular LEGO approach presents a novel method to obtain flexible electronics in a lock-and-key plug and play manner with reliable interconnects. A process of converting standard rigid IC into flexible LEGO without any performance degradation with a high-yield is shown. For the majority of healthcare and other monitoring applications in IoT, sensory array is used for continuous monitoring and spatiotemporal mapping activities. Here we present ultra-high-density sensory solution (1 million sensors) as an epitome of density and address each of the associated challenges. A generic heterogeneous integration scheme has been presented to obtain physically flexible standalone electronic system using 3D-coin architecture. This 3D-coin architecture hosts sensors on one side, readout circuit and data processing units embedded in the polymer, and the other side is reserved for antenna and energy harvester (photovoltaic). This thin platform (~ 300 μm) has achieved bending radius of 1 mm while maintaining reliable electrical interconnection using through-polymer-via (TPV) and soft-polymeric encapsulation. This coin integration scheme is compatible with existing CMOS technology and suitable for large scale manufacturing. Lastly, a featherlight non-invasive ‘Marine-Skin’ platform to monitor deep-ocean monitoring is presented using the heterogeneous integration scheme. Electrical and mechanical characterization has been done to establish reliability, integrity, robustness, and ruggedness of the processes, sensors, and multisensory flexible system.

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Multi-component soft materials offer innovative solutions for traditional and emerging technologies by possessing unique combinations of tunable functionality and adaptive mechanical response. These materials often incorporate functional inclusions such as metals or ceramics in elastomers to create deformable composite structures with high thermal or electrical conductivities, magnetic material response, or stimuli-responsive shape and rigidity tuning. In recent years, these materials have become enabling for wearable electronics and soft machines which has led to the development of new material architectures that provide advanced functionalities while maintaining a low mechanical modulus and high extensibility. In this work, we develop methods for the fabrication and utilization of advanced material architectures which integrate room temperature liquid metals (LM), low melting point alloys (LMPA), and magnetic powders and fluids with soft elastomers to introduce multifunctionality to electronic and machine systems. LM-elastomer composites which have high thermal and electrical conductivities are enabling for heat transfer applications and soft, extensible wiring for wearable electronics and soft robots. These materials have been utilized to create emerging devices such as electronics that are capable of improving human health and efficiency, as well as robots capable of adapting their functions based on environmental need. One possible area where LM composites could be applied is in marine environments, where wearable electronics can improve safety for divers, and soft machines could be utilized for underwater exploration. In Chapter 2, we provide the first study to quantify the effects of underwater aging in freshwater and saltwater environments on the important mechanical and functional properties of LM composites for long-term underwater use. It is found that LM composites are largely resistant to changes in their mechanical properties, as well as both thermal and electrical functionality due to long-term underwater aging. In Chapter 3, we introduce a new chemical approach for the tough bonding of LM composites to diverse substrates, which increases adhesion by up to 100x, improving the integration of these materials with rigid electronics. It is shown that the fracture energy and thermal conductivity of these materials can be tuned by controlling the size and volume loading of the LM inclusions. The utility of this method is then shown through the permanent bonding of LM composites to rigid electronics for use as thermal interface materials. \\ Chapter 4 introduces a multi-component shape morphing material that leverages an LMPA endoskeleton and soft LM resistive heaters to produce rapid (< 0.1 s) and reversible shape change. The morphing material utilizes a unique 'reversible plasticity' mechanism enabled by patterned kirigami cuts that allows for instantaneous shape fixing into load bearing shapes without the need for sustained power. The material properties are enabling for the creation of shape morphing robots, which we show through by integration of on board power and control to create a multi-modal morphing drone capable of land and air transport as well as through an underwater machine that can be reversibly deployed to obtain cargo. For magnetic elastomers, the magneto-mechanical properties of state-of-the-art magnetorheological elastomers (MREs) with diverse structures are studied. These materials have long been studied for their ability to rapidly tune stiffness in the presence of a magnetic field. Chapter 5 introduces a new form of hybrid MRE material architecture which utilizes a combination of magnetic powders and fluids to achieve high magnetic permeability and low stiffness for wearable electronic applications. The zero-field magneto-mechanical properties of MREs with rigid particles, magnetic fluids, and a combination of the two are studied. The inclusions are modeled through an Eshelby analysis which demonstrates magnetic fluids can be utilized to increase magnetic response while decreasing the stiffness of the composite material. The stiffness tuning capabilities of these material architectures are then explored in Chapter 6, where we introduce a predictive model that captures the stiffness tuning response of MREs across diverse microstructures and compositions. This model guides the creation of materials with rapid (~ 20 ms) and extreme stiffness tuning (70x) which we utilize to create a soft adaptive gripper capable of handling objects of diverse geometries. / Doctor of Philosophy / Multi-component soft materials offer innovative solutions for traditional and emerging technologies by possessing unique combinations of tunable functionality and adaptive mechanical properties. These materials often incorporate functional inclusions such as metals or ceramics in elastomers in order to create deformable composite structures with high thermal or electrical conductivities, magnetic material response, or user-controlled shape morphing and stiffness change. In recent years, these materials have become enabling for wearable electronics and soft machines which has led to the development of new materials that provide advanced functionalities while maintaining a low stiffness and high extensibility. In this work, we develop methods for the fabrication and utilization of advanced materials that integrate room temperature liquid metals (LM), low melting point alloys (LMPA), and magnetic powders and fluids with soft elastomers to introduce multifunctionality to electronic and machine systems. LM-elastomer composites which have high thermal and electrical conductivities are enabling for heat transfer and stretchable electronic applications for wearable electronics and soft robots. These materials have been utilized to create emerging devices such as electronics that are capable of improving human health and efficiency, as well as robots capable of adapting their functions based on environmental need. One possible area where LM composites could be applied is in marine environments, where wearable electronics can improve safety for divers, and soft robots could be utilized for underwater exploration. In Chapter 2, we provide the first study to quantify the effects of underwater aging in freshwater and saltwater environments on the important mechanical and functional properties of LM composites for long-term underwater use. It is found that LM composites are largely resistant to changes in their mechanical properties, as well as both thermal and electrical functionality due to long-term underwater aging. In Chapter 3, we introduce a new chemical approach for the tough bonding of LM composites to diverse substrates, which increases adhesion by up to 100x, improving the integration of these materials with rigid electronics. It is shown that the adhesion and thermal conductivity of these materials can be tuned by controlling the size and volume loading of the LM inclusions. The utility of this method is then shown through the permanent bonding of LM composites to rigid electronics for use as thermal interface materials. Chapter 4 introduces a multi-component shape morphing material that leverages an LMPA endoskeleton and soft LM resistive heaters to produce rapid (< 0.1 s) and reversible shape change. The morphing material utilizes a unique 'reversible plasticity' mechanism enabled by patterned kirigami cuts that allows for instantaneous shape fixing into load bearing shapes without the need for sustained power. The material properties are enabling for the creation of shape morphing robots, which we show through by integration of on board power and control to create a multi-modal morphing drone capable of land and air transport as well as through an underwater machine that can be reversibly deployed to obtain cargo. For magnetic elastomers, the magnetic and mechanical properties of state-of-the-art magnetorheological elastomers (MREs) with diverse structures are studied. These materials have long been studied for their ability to rapidly change stiffness in the presence of a magnetic field. Chapter 5 introduces a new form of hybrid MRE material architecture which utilizes a combination of magnetic powders and fluids to achieve exceptional magnetic properties and low stiffness for wearable electronic applications. The mechanical properties of MREs with rigid particles, magnetic fluids, and a combination of the two are studied. The inclusions are modeled through a mechanical analysis which demonstrates magnetic fluids can be utilized to increase magnetic character while decreasing the stiffness of the composite material. The stiffness tuning capabilities of these material architectures are then explored in Chapter 6, where we introduce a predictive model that captures the stiffness tuning response of MREs across diverse microstructures and compositions. This model guides the creation of materials with rapid (~ 20 ms) and extreme stiffness tuning (70x) which we utilize to create a soft adaptive gripper capable of handling objects of diverse geometries.

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