A novel method is established for permittivity enhancement of a silicone matrix for dielectric elastomer actuators (DEAs) by molecular level modifi cations of the elastomer matrix. A push-pull dipole is synthesized to be compatible with the silicone crosslinking chemistry, allowing for direct grafting to the crosslinker molecules in a one-step fi lm formation process. This method prevents agglomeration and yields elastomer fi lms that are homogeneous down to the molecular level. The dipole-to-silicone network grafting reaction is studied by FTIR. The chemical, thermal, mechanical and electrical properties of fi lms with dipole contents ranging from 0 wt% to 13.4 wt% were thoroughly characterized. The grafting of dipoles modifi es the relative permittivity and the stiffness, resulting in the actuation strain at a given electrical fi eld being improved by a factor of six.

Electroactive polymers can be used for actuators with many desirable features, including high electromechanical energy density, low weight, compactness, direct voltage control, and complete silence during actuation. These features may enable personalized robotics with much higher ability to delicately manipulate their surroundings than can be achieved with currently available actuators; however, much work is still necessary to enhance the electroactive materials. Electric field‐driven actuator materials are improved by an increase in permittivity and by a reduction in stiffness. Here, a synergistic enhancement method based on a macromolecular plasticizing filler molecule with a combination of both high dipole moment and compatibilizer moieties, synthesized to simultaneously ensure improvement of electromechanical properties and compatibility with the host matrix is presented. Measurements show an 85% increase in permittivity combined with 290% reduction in mechanical stiffness. NMR measurements confirm the structure of the filler while DSC measurements confirm that it is compatible with the host matrix at all the mixture ratios investigated. Actuation strain measurements in the pure shear configuration display an increase in sensitivity to the electrical field of more than 450%, confirming that the filler molecule does not only improve dielectric and mechanical properties, it also leads to a synergistic enhancement of actuation properties by simple means.

Dielectric elastomer actuators (DEAs) draw their function from their dielectric and mechanical properties. The paper describes the fabrication and various properties of molecularly grafted silicone elastomer films. This was achieved by addition of high-dipole molecular co-substituents to off-the-shelf silicone elastomer kits, Elastosil RT 625 and Sylgard 184 by Wacker and Dow Corning, respectively. Strong push-pull dipoles were chemically grafted to both polymer networks during a one step film formation process. All manufactured films were characterized using (13) C-NMR and FT-IR spectroscopy, confirming a successful attachment of the dipoles to the silicone network. Differential scanning calorimetry (DSC) results showed that grafted dipoles were distributed homogeneously throughout the material avoiding the formation of nano-scale aggregates. The permittivity increased with the amount of dipole at all frequencies, while the Young's modulus and electrical breakdown strength were reduced. Actuation strain measurements in the pure shear configuration independently confirmed the increase in electromechanical sensitivity. The ability to enhance electromechanical properties of off-the-shelf materials could strongly expand the range of actuator properties available to researchers and end-users

The properties of dielectric elastomer actuators can be optimized by modifying the dielectric or mechanical properties of the dielectric elastomer. This paper presents the simultaneous control of both dielectric and mechanical properties, in a silicone elastomer network comprising cross-linker, chains and grafted molecular dipoles. Chains with two different molecular weights were each combined with varying amounts of grafted dipole. Chemical and physical characterization showed that networks with stoichiometric control of cross-linking density and permittivity were obtained, and that longer chain lengths resulted in higher electrical field response due to the reduction in cross-linking density and correspondingly in mechanical stiffness. Both actuation sensitivities were enhanced by 6.3 and 4.6 times for the short and long chain matrix material, respectively.

Silicone elastomers are highly suitable for application in the field of dielectric elastomer actuators (DEA) due to their unique material properties (e.g. low glass temperature, thermal stability, large capability of chemical tailoring). The elastomer forming Polydimethysiloxane (PDMS) employed for this study consists of chains with vinyl termination and is cross linked via hydrosilylation to a cross linking molecule in the presence of platinum catalyst. Here, dipole molecules (N-Allyl-N-methyl-4-nitroaniline) were specifically synthesized such that they could chemically graft to the silicone network. The most prominent advantage of this approach is the achievement of a homogeneous distribution of dipoles in the PDMS matrix and a suppression of phase separation due to the grafting to the junction points of the rubber network. Several films with dipole contents v ranging from 0 % wt up to 10.9 % wt were prepared. The films were investigated to determine their mechanical (tensile testing), dielectric (dielectric relaxation spectroscopy) and electrical (electrical breakdown) properties. This new approach for composites on the molecular level leads to homogeneous films with enhanced material properties for DEA applications. An increase in permittivity from 3.3 to 6.0, a decrease in electrical breakdown from 130 V/μm to 50 V/μm and a lowering of the mechanical stiffness from 1700 kPa to 300 kPa was observed. © 2011 SPIE

An instrument is described, which measures the efficiency of Förster resonance energy transfer (FRET) in parallel to the sample's turbidity. The instrument was used to study the film formation from polymer latex dispersions. In this context, the FRET efficiency reflects the diffusion of polymer chains across the interparticle boundaries, while the loss of turbidity reflects the progress of particle deformation. Particle deformation causes tensile in-plane stress, while polymer interdiffusion creates cohesion and thereby helps to prevent cracking. The relative timing between the two therefore is of fundamental importance for successful film formation. The on-line determination of FRET efficiency while the film dries is complicated by the fact that the fluorescence lifetime of the donor, τ(D), depends on the water content in the vicinity of the donor. In the established procedure for data analysis, drifts in τ(D) induce corresponding artifical drifts in the values of the FRET efficiency. A novel algorithm for the analysis of fluorescence decay profiles is proposed, which makes use of the method of moments. The FRET efficiency is quantified by the upward curvature of the fluorescence decay curve in log-linear display. In the application example, interdiffusion is delayed relative to particle deformation by about 10 min. For successful film formation, this delay should be as small as possible.

Dielectric elastomer actuators (DEAs) can be optimized by modifying the dielectric or mechanical properties of the electroactive polymer. In this work both properties were improved simultaneously by a simple process, the one-step film formation for polyurethane and silicone films. The silicone network contains polydimethylsiloxane (PDMS) chains, as well as cross-linker and grafted molecular dipoles in varying amounts. The process leads to films, which are homogenous down to the molecular level and show higher permittivities as well as reduced stiffnesses. The dipole modification of a new silicone leads to 40 times higher sensitivities, compared to the unmodified films. This new material reaches the sensitivity of the widely used acrylate elatomer VHB4905. A similar silicone modification was obtained by using smart fillers consisting of organic dipoles and additional groups realizing a high compatibility to the silicon network. Polyurethanes are alternative elastomers fo r DEAs which are compared with the silicones in important properties. Polyurethanes have an intrinsically high dielectric constant (above 7), which is based on the polar nature of the polyurethane fragments. Polyurethanes can be made in roll-to-roll process giving constant mechanical and electrical properties on a high level

Dielectric elastomer actuators (DEAs) can be optimized by modifying the dielectric or mechanical properties of the electroactive polymer. In this work both properties were improved simultaneously by a simple process, the one-step film formation. The silicone elastomer network contains polydimethylsiloxane (PDMS) chains, as well as crosslinker and grafted molecular dipoles in varying amounts. This leads to films, which are homogenous down to the molecular level. Films with higher permittivity and reduced stiffness were obtained. As matrix two PDMS-materials with different molar masses, leading to other network chain lengths, were compared. This directly influences the network density and thus the mechanical properties. A higher electrical field response for long chain matrix materials was found. The actuation sensitivities for both materials were enhanced by 6.3 and 4.6 times for the short and long chain matrix material, respectively