Dielectric elastomers are electroactive polymers, which change size and shape in response to an electrical field. Dielectric elastomer actuators (DEAs) are highly promising new technologies in optical applications such as tuneable optical lenses, diffraction gratings and active camouflage. This thesis aims to develop a new approach to create a strain actuated compliant colour changing device that is controlled using DEAs as they offer stretchability, low weight, high efficiency, low cost and the possibility for miniaturisation. Conventional DEAs use transparent elastomeric materials with no significant colour change with strain. Conversely, liquid crystal materials are known to display dynamic colour changing behaviour, thereby making them good candidate materials. The thesis examines both the potential for colour changing soft actuators and the upcoming challenges in this field as well as the key concepts around liquid crystals that exhibit colour change. An initial approach was aimed at creating colour changes using dielectric elastomer actuators that drove a masked positioner. This method showed colour change since the mask changes the colour visualisation. The second approach used polymer dispersed liquid crystals, such as a nematic liquid crystal within a reactive silicone resin. The immiscibility of these compounds resulted in a dispersion of the liquid crystal droplets in the silicone matrix. However, the optical properties could not be controlled through mechanical deformation alone and the alignment of resulting LC droplets in the PDLC films was sensitive to the substrate used to perform the actuation. The next approach used reactive cholesteric liquid crystals (CLC) instead. A thin film coating process was preferred to carefully control the film's thickness by stretching. In free standing films a planar cholesteric alignment was obtained with mesogens aligned parallel to the substrate and colour was achieved based on the selective reflection of light. A transfer print technique was introduced to combine CLC coatings with elastomeric substrates that can be stretched. However, no colour change was achieved in response to mechanical deformation primarily due to the modulus and strength mismatch between the thin film and the elastomeric susbstrate material. Finally, lightly crosslinked liquid crystal elastomers using a combination of reactive and non-reactive liquid crystals were produced that were compatible with elastomer substrate materials. In free standing films planar cholesteric alignment was obtained with mesogens aligned parallel to the substrate. Successfully a reversible colour change based on selective reflection of light was achieved in response to a mechanical deformation.

Electro-active polymers (EAPs) have emerged as a new class of active materials, which produce large deformations in response to an electric stimulus. EAPs have attractive characteristics of being lightweight, inexpensive, stretchable, and flexible. Additionally, EAPs are conformable, and their properties can be tailored to satisfy a broad range of requirements. These advantages have enabled many target applications in actuation and sensing. A general constitutive formulation for isotropic and anisotropic electro-active materials is developed using continuum mechanics framework and invariant theory. Based on the constitutive law, electromechanical stability of the electro-elastic materials is investigated using convexity and polyconvexity conditions. Implementation of the electro-active material model into a commercial finite element software (ABAQUS 6.9.1, PAWTUCKET, RI, USA) is presented. Several boundary and initial value problems are solved to investigate the actuation and sensing response of isotropic and anisotropic dielectric elastomers (DEs) subject to combined mechanical and electrical loads. The numerical response is compared with experimental results to validate the theoretical model. For the constitutive formulation of the electro-elastic materials, invariants for the coupling between two families of electro-active fibers (or particles) and the applied electric field are introduced. The effect of the orientation of the electro-active fibers and the electric field on the electromechanical coupling is investigated under equibiaxial extension. Advantage of the constitutive formulation derived in this research is that the electromechanical coupling can be illustrated easily by choosing invariants for the deformation gradient tensor, the electro-active fibers, and the electric field. For the electromechanical stability, it is shown that the stability can be controlled by tuning the material properties and the orientation of the electro-active fibers. The electromechanical stability condition is useful to build a stable free energy function and prevent the instabilities (wrinkling and electric breakdown) for the electro-elastic materials. The invariant-based constitutive formulation for the electro-elastic materials including the isotropic and anisotropic DEs is implemented into a user subroutine (UMAT in ABAQUS: user defined material) by using multiplicative decomposition of the deformation gradient and the applicability of the UMAT is shown by simulating a complicated electromechanical coupling problem in ABAQUS/CAE. Additionally, the static and dynamic sensing and actuation response of tubular DE transducers (silicone and polyacrylate materials) with respect to combined electrical and mechanical stimuli is obtained experimentally. It is shown that the silicone samples have better dynamic and static sensing characteristics than the polyacrylate. The theoretical modeling accords well with the experimental results. / Ph. D.

Multifunctional Dielectric Elastomer (DE) devices are well established as actuators, sensors and energy harvesters. Since the invention of the Dielectric Elastomer Switch (DES), a piezoresistive electrode that can directly switch charge on and off, it has become possible to expand the wide functionality of DE structures even more. We show the application of fully soft DE subcomponents in biomimetic robotic structures. It is now possible to couple arrays of actuator/switch units together so that they switch charge between themselves on and off. One can then build DE devices that operate as self-controlled oscillators. With an oscillator one can produce a periodic signal that controls a soft DE robot { a DE device with its own DE nervous system. DESs were fabricated using a special electrode mixture, and imprinting technology at an exact pre-strain. We have demonstrated six orders of magnitude change in conductivity within the DES over 50% strain. The control signal can either be a mechanical deformation from another DE or an electrical input to a connected dielectric elastomer actuator (DEA). We have demonstrated a variety of fully soft multifunctional subcomponents that enable the design of autonomous soft robots without conventional electronics. The combination of digital logic structures for basic signal processing, data storage in dielectric elastomer ip-ops and digital and analogue clocks with adjustable frequencies, made of dielectric elastomer oscillators (DEOs), enables fully soft, self-controlled and electronics-free robotic structures. DE robotic structures to date include stiff frames to maintain necessary pre-strains enabling sufficient actuation of DEAs. Here we present a design and production technology for a first robotic structure consisting only of soft silicones and carbon black.

La légèreté, simplicité et robustesse des systèmes mécaniques binaires font en sorte qu'ils sont une alternative prometteuse aux systèmes analogiques employés de nos jours dans des applications en robotique et en mécatronique. Les performances de systèmes mécaniques binaires sont présentement restreintes par la complexité, le poids et le coût des actionneurs conventionnels. De nouvelles technologies d'actionneurs, telles celles des matériaux intelligents (Smart Materials), doivent donc être développées afin de permettre l'essor et la commercialisation de systèmes binaires performants. Les actionneurs diélectriques en polymère (Dielectric Elastomer Actuators : DEA) sont capables de grandes déformations et de hautes énergies volumiques. Toutefois, l'application de cette technologie d'actionneurs à des systèmes binaires concrets est présentement limitée par la faible fiabilité de ces actionneurs et les faibles énergies volumiques développées par les configurations de DEAs actuelles. Afin de permettre l'avancée de la technologie des DEAs dans des applications binaires, cette recherche propose des configurations antagonistes et bistables qui développent ~10x plus d'énergie volumique que les configurations bistables développées antérieurement. De plus, cette recherche investigue les impacts des techniques de fabrication sur la fiabilité des actionneurs.

There is a growing interest in the field of Dielectric Elastomer Actuators (DEAs).A DEA consists of a thin DE lm coated with a compliant electrode. It expandsin planar directions and contracts in thickness under a driving voltage. Becauseof the similar actuation capability compared with human muscles, it is oftenreferred as artificial muscle. One possible application is to integrate the DEA inwearable devices for tremor suppression. In this thesis, the development of theDEA has been advanced towards this application in three aspects: performanceenhancement, modelling accuracy and self-sensing control. The results presented demonstrate that the combination of pre-strain and motion constraining enhances the force output of the DEA significantly but it also leads to the pre-mature electric breakdown that shortens the operational life. This drawback was suppressed by optimising the electrode configuration to avoid the electrically weak regions with low thickness across the DE lm, together with the lead contact o the active electrode region. The durability of the enhanced DEA was therefore improved significantly. Polyacrylate, a commonly used DE, was characterised for dynamic mechanical loading and electrical actuation. The conventional Kelvin-Voigt model was proved to be deficient in simulating the viscoelastic behaviour of polyacrylate in the frequency domain. The error in modelling was substantially reduced using a higher material model that contains multiple spring-damper combinations. It allows the system dynamics to be shaped over frequency ranges. A detailed procedure was given to guide the parameter identification in higher order material model. A novel self-sensing mechanism that does not require superposition of drivingvoltage and excitation signal was also designed. It reconfigures the conventionalDEA to have separate electrode regions for sensing and actuating. As the DElm deforms under driving voltage, the capacitive change in the electrode regionfor sensing was measured via a capacitor bridge and used as the feedback foractuation control. The self-sensing DEA can, therefore, be implemented with anyhigh voltage power supply. Moreover, the sensing performance is demonstratedto have improved consistency without interference of the electrical field. It alsohas a unique feature of DE lm wrinkling detection.

Touch is one of the less exploited sensory channels in human machine interactions. While the introduction of the tactile feedback would improve the user experience in several fields, such as training for medical operators, teleoperation, computer aided design and 3D model exploration, no interfaces able to mimic accurately and realistically the tactile feeling produced by the contact with a real soft object are currently available. Devices able to simulate the contact with soft bodies, such as the human organs, might improve the experience. The existing commercially available tactile displays consist of complex mechanisms that limit their portability. Moreover, no devices are able to provide tactile stimuli via a soft interface that can also modulate the contact area with the finger pad, which is required to realistically mimic the contact with soft bodies, as needed for example in systems aimed at simulating interactions with virtual biological tissues or in robot-assisted minimally invasive surgery. The aim of this thesis is to develop such a wearable tactile display based on the dielectric elastomer actuators (DEAs). DEAs are a class of materials that respond to an electric field producing a deformation. In particular, in this thesis, the tactile element consists of a so-called hydrostatically coupled dielectric elastomer actuator (HC-DEAs). HC-DEAs rely on an incompressible fluid that hydrostatically couples a DEA-based active part to a passive part interfaced to the user. The display was also tested within a closed-loop configuration consisting of a hand tracking system and a custom made virtual environment. This proof of concept system allowed for a validation of the abilities of the display. Mechanical and psychophysical tests were performed in order to assess the ability of the system to provide tactile stimuli that can be distinguished by the users. Also, the miniaturisation of the HC-DEA was investigated for applications in refreshable Braille displays or arrays of tactile elements for tactile maps.

<p>A variety of intriguing surface patterns have been observed on developing natural systems, ranging from corrugated surface of white blood cells at nanometer scales to wrinkled dog skins at millimeter scales. To mimetically harness functionalities of natural morphologies, artificial transformative skin systems by using soft active materials have been rationally designed to generate versatile patterns for a variety of engineering applications. The study of the mechanics and design of these dynamic surface patterns on soft active materials are both physically interesting and technologically important. </p><p>This dissertation starts with studying abundant surface patterns in Nature by constructing a unified phase diagram of surface instabilities on soft materials with minimum numbers of physical parameters. Guided by this integrated phase diagram, an electroactive system is designed to investigate a variety of electrically-induced surface instabilities of elastomers, including electro-creasing, electro-cratering, electro-wrinkling and electro-cavitation. Combing experimental, theoretical and computational methods, the initiation, evolution and transition of these instabilities are analyzed. To apply these dynamic surface instabilities to serving engineering and biology, new techniques of Dynamic Electrostatic Lithography and electroactive anti-biofouling are demonstrated.</p> / Dissertation

Electrical motors and/or hydraulics and pneumatics cylinders are commonly used methods of actuation in mechanical systems. Over the last two decades, due to arising market needs, novel self-independent mobile systems such as mobility assistive devices have emerged with the help of new advancements in technology. The actuation criteria for these devices differ greatly from typical mechanical systems, which has made the implementation of classical actuators difficult within modern assistive devices. Among the numerous challenges, limited energy storage capabilities by mobile systems have restricted their achievable operational time. Furthermore, new expectations for device weight and volume, as well as actuator structural compliance, have added to this quandary. Electroactive polymers, a category of smart materials, have emerged as a strong contender for the use in low-cost efficient actuators. They have demonstrated great potential in soft robotic and assistive device/prosthetic applications due to their actuation potential and similar mechanical behaviour to human skeletal muscles. Dielectric Elastomers, in particular, have shown very promising properties for these types of applications. Their structures have shown large achievable deformation, while remaining light-weight, mechanically efficient, and low-cost. This thesis aims to characterize, and model the behaviour of 3MTM VHB polyacrylic dielectric elastomer, in order to establish a foundation for its implementation in a proposed novel linear actuator concept. In this thesis, a comprehensive experimental evaluation is accomplished, which resulted in the better understanding of the elastomer’s biaxial mechanical and electro-mechanically coupled behaviours. Subsequently, a constitutive biaxial mechanical model was derived in order to provide a predictive design equation for future actuator development. This model proved effective in providing a predictive tool for the biaxial mechanical tensile response of the material. Finally, a simplified prototype was devised as a proof of concept. This first iteration applied experimental findings to validate the working principles behind the proposed actuator design. The results confirmed the proof of concept, through achieved reciprocal linear motion, and provided insight into the design considerations for prototype optimization and final actuator development.

In der vorliegenden Dissertationsschrift wird ein thermo-elektro-mechanisches Modell zur Simulation des Verhaltens von dielektrischen Elastomeraktoren vorgestellt. Zur Beschreibung der elektrischen und thermischen Eigenschaften werden lineare Modelle verwendet. Ein isotropes viskohyperelastisches mechanisches Materialmodell wird auf Grundlage der Hyperelastizität nach Ogden und der Beschreibung viskosen Verhaltens mittels Prony-Reihen eingesetzt. Die elektromechanische Kopplung ist durch die elektrostatische Anziehungskraft geladener Elektroden begründet. Die verlustbehafteten Prozesse der elektromechanischen Energieumwandlung bzw. des Ladungstransports führen zu einer Verlustleistung, welche in Wärme umgewandelt wird. Auf diese Weise wird eine unidirektionale Kopplung zwischen dem elektromechanischen und dem thermischen Feld erreicht. Die entsprechenden Materialparameter wurden der Literatur entnommen oder von Daten experimenteller Untersuchungen abgeleitet, welche am Institut für Elektromechanische Konstruktion (EMK) der Technischen Universität Darmstadt durchgeführt wurden. Mittels der Finite-Elemente-Methode wurde das thermo-elektro-mechanischen Modell zur Simulation zweier Testgeometrien verwendet. Dabei wurde eine gute qualitative Übereinstimmungen zwischen den Ergebnissen der numerisch Simulation und den experimentellen Beobachtungen des EMK erreicht. Die Ursachen quantitativer Differenzen zwischen den experimentell ermittelten und den numerisch berechneten Temperaturen werden untersucht und diskutiert. Abgeleitet aus den Ergebnissen der numerischen Untersuchungen werden abschließend Vorschläge zu einer Verringerung der dissipationsbedingten Erwärmung unterbreitet. Diese Vorschläge sind durch konstruktive, beispielsweise geometrische oder materielle, Eigenschaften von DE-Aktoren begründet, oder können aufgrund der aktiven Anregung getroffen werden.

Silicone stands as an indispensable material for numerous applications; however, its high energy-cost synthesis poses significant environmental challenges. To address these concerns, bio-based silicone has gained considerable attention, showcasing its potential to dilute energy density while offering inherent functional benefits. Despite promising prospects, existing incorporation methods often involve protecting groups, rare metal catalysts, and multistep synthesis, which contradict green chemistry principles. The aza- Michael reaction emerges as a superior choice due to its high atom economy and mild reaction conditions. However, it still suffers from prolonged reaction times, hindering its overall efficiency and sustainability. This thesis utilizes self-activated beta-hydroxy acrylates to greatly enhance aza-Michael kinetics, achieving a 3-fold rate enhancement in solvent-free silicone synthesis. This fast aza-Michael reaction acts as the platform for the incorporation of Vitamin C and amino acids into silicone materials. Vitamin C-modified silicone demonstrates the potential for controlled antioxidant activity release, while amino acid-functionalized silicones are synthesized using choline amino acid ionic liquids, presenting a protecting-group-free and solvent-free synthesis method. Moreover, the synthesized choline amino acid-functional polymers and elastomers are investigated for their dielectric properties revealing promising potential for dielectric elastomer actuator applications. These innovative methods offer green alternatives for incorporating hydrophilic biomolecules into hydrophobic silicone systems, providing new functionalities that address both environmental and functional requirements. / Thesis / Doctor of Science (PhD)