Nematic Elastomers Research Articles

Overdamping of vibration resonances by liquid crystal elastomers

This work aims to compare the capability of vibration attenuation by standard elastomeric polymers, and by the new anomalously damping nematic liquid crystal elastomer. We use the most mainstream materials in both categories, and design two testing platforms: the ASTM-standard constrained layer plate resonance geometry, and the attenuation of resonances in a commercial device (electric drill) where the damping polymers were inserted into the casing. In the standard plate resonance testing, we find that LCE outperforms all standard damping materials, moreover, it brings the vibrating plate into the overdamped condition, which is unique for a non-fluid dissipative system. In the attenuation of high-frequency vibrations of a device, we also found LCE dissipates these vibrations much better, although we did not find the optimal insertion configuration for the damping polymer, and did not reach overdamping.

Adhesion of a nematic elastomer cylinder.

Reversible dry adhesion is exploited by lizards and insects in nature, and is of interest to robotics and bio-medicine. In this paper, we use numerical simulation to study how the soft elasticity of liquid crystal elastomers can affect its adhesion and provide a technological opportunity. Liquid crystal elastomers are cross-linked elastomer networks with liquid crystal mesogens incorporated into the main or side chain. Polydomain liquid crystalline (nematic) elastomers exhibit unusual mechanical properties like soft elasticity, where the material deforms at nearly constant stress, due to the reorientation of mesogens. Our study reveals that the soft elasticity of nematic elastomers dramatically affects the interfacial stress distribution at the interface of a nematic elastomer cylinder adhered to a rigid substrate. The stress near the edge of the nematic cylinder under tensile load deviates from the singular behavior predicted for linear elastic materials, and the maximum normal stress reduces dramatically. This suggests that nematic elastomers should display extremely high, but controllable adhesion, consistent with the available experimental observations.

Effects of carbon nanotubes on the isotropic to nematic phase transition in nematic liquid crystal elastomer

The isotropic to nematic phase transition on nematic liquid crystal elastomer - carbon nanotubes composites has been studied theoretically. The model free energy density has been constructed using Flory Huggins theory of isotropic mixing and Landau-de Gennes theory. The effects of carbon nanotubes and external mechanical stress on the isotropic to nematic phase transition of the nematic liquid crystal elastomer-carbon nanotubes composites have been discussed. The volume fraction of carbon nanotubes dependence of the isotropic to nematic transition temperature, mechanical strain and strain birefringence has been calculated. The weak first-order character of the isotropic to nematic phase transition on nematic liquid crystal elastomer-carbon nanotubes composites has been predicted.

A hyperelastic beam model for the photo-induced response of nematic liquid crystal elastomers

Liquid crystal elastomers (LCEs) are a novel class of materials created by combining polymeric solids with stiff, rod-like molecules known as nematic mesogens. These materials exhibit large, reversible deformations under mechanical, thermal, and optical stimuli. In this work, we develop a nonlinear beam formulation for analyzing the finite elastic deformation of beam-like structures made of LCEs under photo-actuation. This formulation applies to ideal, non-ideal, isotropic genesis, and nematic genesis LCEs. We establish the variational form of the problem based on the principle of virtual work. To solve numerical examples, we also develop a nonlinear finite element formulation based on B-spline functions. Several numerical examples are presented to demonstrate the applicability of the proposed formulation.

Theoretical and experimental study of elastocaloric responses in liquid crystalline elastomers

We carry out systematic experimental and theoretical study of elastocaloric (eC) response in nematic liquid crystal elastomers (LCEs), which possess the elastic properties of elastomers combined with the orientational order of liquid crystals. The chemical linking of mesogens to the polymer backbone enables thermomechanical response yielding a large spontaneous change in the LCE geometry on varying the temperature. In LCEs, a relatively large eC effect could be obtained upon adiabatic application or removal of a stress field in the isotropic state near phase transformation to the more ordered state. In these cases a change in the isothermal entropy or adiabatic temperature is compensated with the temperature change of liquid crystal elastomers. This effect could be exploited towards soft condensed state cooling technologies that gain increasing interest due to environmental issues, low-cost and low stimuli field. In the present study we measure directly the elastocaloric temperature change. Experimental measurements are interpreted using a modified Landau-de Gennes mesoscopic model taking into account both internal and external stress fields. Our systematic study identifies conditions yielding responsivity of a few K/MPa, which is two orders of magnitude larger than in the shape memory alloys, the most intensively studied materials for this effect.

Creasing instability of polydomain nematic elastomers in compression

Polydomain liquid crystalline (nematic) elastomers exhibit unique mechanical properties such as soft elasticity, where the material largely deforms at nearly constant stress, due to microstructural evolution. In this paper, we numerically study the effect of such remarkable soft behavior on the surface instability of a half-space polydomain nematic elastomer, which is uniformly compressed parallel to the interface under a plane-strain condition. We compare the creasing instability of nematic elastomers with that of neo-Hookean elastomers by presenting bifurcation diagrams, stress and strain development in the elastomers, energy relaxation, and surface morphology at the creased state. Our results reveal that soft elasticity stabilizes nematic elastomers in plane-strain compression. Remarkably, the critical strain and stress at which the crease nucleates depend nonlinearly on the degree of anisotropy in nematic elastomers. Moreover, we find that the morphology of the creased surface in nematic elastomers exhibits the universal cusp shape previously observed in neo-Hookean elastomers.

Simulating loading–unloading hysteretic behaviors of nematic-genesis polydomain nematic elastomers

Nematic elastomers (NEs) are lightly cross-linked elastomers with nematic mesogens integrated in their polymer networks. Combination of large deformation capability with nematic-isotropic phase transition enables NEs to be the most promising soft materials for impact attenuation, actuation and soft robotics. In this paper, we focus on nematic-genesis polydomain NEs (N-PNEs) where mesogens are cross-linked at nematic states. N-PNEs are capable of absorbing and dissipating energy and easy to synthesize. We present a Voronoi diagram-based finite element model for specimen-scale N-PNEs, and investigate the cyclic tensile and compressive behaviors of N-PNEs at different strain rates. Our simulations reveal a smooth polydomain-monodomain transition during loading, accompanied by a full recovery of polydomain texture after the load is removed, indicating a memory effect of initial disordered mesogen alignment. The predicted behaviors align well with experimental observations, which validates our model. Furthermore, we assess the energy absorption and dissipation capabilities of N-PNEs compared to monodomain NEs, identifying conditions where N-PNEs exhibit superior performance. This study not only enhances our understanding of polydomain-monodomain transitions in N-PNEs, but also lays the groundwork for the development of N-PNE-based energy absorbers.

Mesogen Organizations in Nematic Liquid Crystal Elastomers Under Different Deformation Conditions.

Liquid crystal elastomers (LCEs) exhibit unique mechanical properties of soft elasticity and reversible shape-changing behaviors, and so serve as potentially transformative materials for various protective and actuation applications. This study contributes to filling a critical knowledge gap in the field by investigating the microscale mesogen organization of nematic LCEs with diverse macroscopic deformation. A polarized Fourier transform infrared light spectroscopy (FTIR) tester is utilized to examine the mesogen organizations, including both the nematic director and mesogen order parameter. Three types of material deformation are analyzed: uniaxial tension, simple shear, and bi-axial tension, which are all commonly encountered in practical designs of LCEs. By integrating customized loading fixtures into the FTIR tester, mesogen organizations are examined across varying magnitudes of strain levels for each deformation mode. Their relationships with macroscopic stress responses are revealed and compared with predictions from existing theories. Furthermore, this study reveals unique features of mesogen organizations that have not been previously reported, such as simultaneous evolutions of the mesogen order parameter and nematic director in simple shear and bi-axial loading conditions. Overall, the findings presented in this study offer significant new insights for future rational designs, modeling, and applications of LCE materials.

Thermally Generated Isometric Stress Performances of Polydomain and Monodomain Nematic Elastomers

Thermally Generated Isometric Stress Performances of Polydomain and Monodomain Nematic Elastomers

On the effect of strain rate during the cyclic compressive loading of liquid crystal elastomers and their 3D printed lattices

Nematic liquid crystal elastomers (LCEs) are a unique class of network polymers with the potential for enhanced mechanical energy absorption and dissipation capacity over conventional network polymers because they exhibit both conventional viscoelastic behavior and soft-elastic behavior (nematic director changes under shear loading). This additional inelastic mechanism makes them appealing as candidate damping materials in a variety of applications from vibration to impact. The lattice structures made from the LCEs provide further mechanical energy absorption and dissipation capacity associated with packing out the porosity under compressive loading.Understanding the extent of mechanical energy absorption, which is the work per unit mass (or volume) absorbed during loading, versus dissipation, which is the work per unit mass (or volume) dissipated during a loading cycle, requires measurement of both loading and unloading response. In this study, a bench-top linear actuator was employed to characterize the loading-unloading compressive response of polydomain and monodomain LCE polymers and polydomain LCE lattice structures with two different porosities (nominally, 62% and 85%) at both low and intermediate strain rates at room temperature. As a reference material, a bisphenol-A (BPA) polymer with a similar glass transition temperature (9 °C) as the nematic LCE (4 °C) was also characterized at the same conditions for comparing to the LCE polymers. Based on the loading-unloading stress-strain curves, the energy absorption and dissipation for each material at different strain rates (0.001, 0.1, 1, 10 and 90 s-1) were calculated with considerations of maximum stress and material mass/density. The strain-rate effect on the mechanical response and energy absorption and dissipation behaviors was determined. The energy dissipation ratio was also calculated from the resultant loading and unloading stress-strain curves. All five materials showed significant but different strain rate effects on energy dissipation ratio. The solid LCE and BPA materials showed greater energy dissipation capabilities at both low (0.001 s−1) and high (above 1 s−1) strain rates, but not at the strain rates in between. The polydomain LCE lattice structure showed superior energy dissipation performance compared with the solid polymers especially at high strain rates.

Generalized continuum theory for nematic elastomers: Non-affine motion and characteristic behavior

We develop a physically-motivated mechanical theory for predicting the behavior of nematic elastomers — a subset of liquid crystal elastomers (LCEs). We begin with a statistical description of network geometry that naturally incorporates independent descriptors for the mesogens, which create the nematic phase, and the polymer chains, which are assumed to not deform affinely with global deformations. From here, we develop thermodynamically consistent constitutive laws based on classical continuum mechanics principles and ultimately provide simple governing equations with transparent physical interpretation. We found that our framework converges identically to two previously developed mechanical theories, including the well-known neo-classical theory, when considering the extreme ends of our parametric space. We then explore the new predictive capabilities of our model inside these two extremes and illustrate its unique predictions at finite strains, which are distinct in form from other theories. We validate our model using published experimental data from four monodomain nematic liquid crystal elastomers.

Dynamic large strain formulation for nematic liquid crystal elastomers

Liquid crystal elastomers (LCEs) are a class of materials which exhibit an anisotropic behavior in their nematic state due to the main orientation of their rod-like molecules called mesogens. The reorientation of mesogens leads to the well-known actuation properties of LCEs, i.e. exceptionally large deformations as a consequence of particular external stimuli, such as temperature increase. Another key feature of nematic LCEs is the capability to undergo deformation by constant stresses while being stretched in a direction perpendicular to the orientation of mesogens. During this plateau stage, the mesogens rotate towards the stretching direction. Such characteristic is defined as semisoft elastic response of nematic LCEs. We aim at modeling the semisoft behavior in a dynamic finite element method based on a variational-based mixed finite element formulation. The reorientation process of the rigid mesogens relative to the continuum rotation is introduced by micropolar drilling degrees of freedom. Responsible for the above-mentioned characteristics is an appropriate free energy function. Starting from an isothermal free energy function based on the small strain theory, we aim to widen it into the framework of large strains by identifying tensor invariants. In this work, we analyze the isothermal influence of the tensor invariants on the mechanical response of the finite element formulation and show that its space-time discretization preserves mechanical balance laws in the discrete setting.

Effects of Operating Mechanical Conditions and Polymer Networks of Nematic Elastomers on Photo-Induced Mechanical Performances.

Photoresponsive liquid-crystalline elastomers (LCEs) are promising candidates for light-controlled soft actuators. Photoinduced stress/strain originates from the changes in mechanical properties after light irradiation. However, the correlation between the photoinduced mechanical performance and in-use conditions such as stress/strain states and polymer network properties (such as effective crosslink density and dangling chain density) remains unexplored for practical applications. Here, isometric photo-induced stress or isotonic strain is investigated at different operating strains or stresses, respectively, on LCEs with polymer network variations, produced by different amounts of solvent during polymerization. As the solvent volume increases, the moduli and photoinduced stresses decrease. However, the photo-induced strain, fracture strain, fracture stress, and viscosity increase. The optical response performance initially increases with the operating strain/stress, peaks at a higher actuation strain/stress, and then, decreases depending on the polymer network. The maximum work densities, which also depend on the operating stress, are in the range of ≈200-300 kJm-3. These findings, highlighting the significant variations in the mechanical performance with the operating stress/strain ranges and amount of solvent used in the synthesis, are critical for designing LCE-based mechanical devices.

Coupling between viscoelasticity and soft elasticity in main-chain nematic Liquid Crystal Elastomers

Liquid crystal elastomers (LCEs) are a class of smart elastomers exhibiting unusual mechanical behavior, including large energy dissipation and soft elasticity under uniaxial tensile loading. LCEs are composed of liquid crystal molecules, called mesogens, linked by a network of polymer chains. During deformation, the mesogens orient in the direction of the loading, leading to soft elasticity, which is an increase in strain at constant stress. The combination of mesogen rotation and intrinsic polymer viscoelasticity leads to a nonlinear viscoelastic soft elastic behavior. The aim of this paper is to investigate the coupling between the viscoelastic mechanisms and soft elasticity in main chain LCEs. We propose a rheological model in which the mesogen rotation during deformation is represented by a reversible slider while viscoelastic relaxation mechanisms are modeled as series of Maxwell elements coupled or decoupled with mesogen rotation. Fitting this model to experimental data demonstrate that the coupling between polymer chain viscoelasticity and mesogen rotation is partial, i.e. the long-time relaxation mechanisms are coupled and the short-time relaxation mechanisms are decoupled from mesogen rotation. Furthermore, we show that the viscosity of mesogen rotation is not necessary to properly predict the elastic modulus during the soft elasticity but it is needed to properly predict the initiation of the phenomenon.

Revealing the unusual rate-dependent mechanical behaviors of nematic liquid crystal elastomers

Liquid crystal elastomers (LCEs) exhibit unique mechanical properties of soft elasticity and enhanced energy dissipation with rate dependency. They are potentially transformative materials for applications in mechanical impact mitigation and vibration isolation. However, previous studies have primarily focused on the mechanics of LCEs under equilibrium and quasistatic loading conditions. Critical knowledge gaps exist in understanding their rate-dependent behaviors, which are a complex mixture of traditional network viscoelasticity and the soft elastic behaviors with changes in the mesogen orientation and order parameter. Together, these inelastic mechanisms lead to unusual rate-dependent energy absorption responses of LCEs. In this work, we developed a viscoelastic constitutive theory for monodomain nematic LCEs to investigate how multiple underlying sources of inelasticity manifest in the rate-dependent and dissipative behaviors of monodomain LCEs. The theoretical modeling framework combines the neo-classical network theory with evolution rules for the mesogen orientation and order parameter with conventional viscoelasticity. The model is calibrated with uniaxial tension and compression data spanning six decades of strain rates. The established 3D constitutive model enables general loading predictions taking the initial mesogen orientation and order parameter as inputs. Additionally, parametric studies were performed to further understand the rate dependence of monodomain LCEs in relation to their energy absorption characteristics. Based on the parametric studies, particularly loading scenarios are identified as conditions where LCEs outperform conventional elastomers regarding energy absorption.

Surface Instability in a Nematic Elastomer.

Liquid crystal elastomers (LCEs) are soft phase-changing solids that exhibit large reversible contractions upon heating, Goldstone-like soft modes, and resultant microstructural instabilities. We heat a planar LCE slab to isotropic, clamp the lower surface, then cool back to nematic. Clamping prevents macroscopic elongation, producing compression and microstructure. We see that the free surface destabilizes, adopting topography with amplitude and wavelength similar to thickness. To understand the instability, we numerically compute the microstructural relaxation of a "nonideal" LCE energy. Linear stability reveals a Biot-like scale-free instability, but with oblique wave vector. However, simulation and experiment show that, unlike classic elastic creasing, instability culminates in a crosshatch without cusps or hysteresis, and is constructed entirely from low-stress soft modes.

Modeling the thermo-responsive behaviors of polydomain and monodomain nematic liquid crystal elastomers

Liquid crystal elastomers (LCEs) are polymeric materials that combine liquid crystal orientation and rubber elasticity. The mechanical responses of LCEs strongly depend on the nematic order and temperature. Developing a thermo-order-mechanical coupling model is important for the engineering applications of LCEs. In this work, we first synthesize both polydomain and monodomain LCEs. The shape change with temperature under a certain stress level is further characterized. In the theoretical part, the Landau–de Gennes model and neo-classical model are combined to construct the free energy density of LCEs. A linear term accounting for the effect of interior stress on nematic–isotropic transition is incorporated into the Landau–de Gennes free energy density, while a macro-order parameter is defined to describe the polydomain–monodomain transition for polydomain LCEs induced by the external force. Comparison between the model predictions and experimental results shows acceptably consistency for both polydomain and monodomain LCEs. Therefore, this work provides an efficient approach to predict the shape change of LCEs in various scenarios.

Controllable Deformations of Unconstrained Ideal Nematic Elastomers

We establish that, for ideal unconstrained uniaxial nematic elastomers described by a homogeneous isotropic strain-energy density function, the only smooth deformations that can be controlled by the application of surface tractions only and are universal in the sense that they are independent of the strain-energy density are those for which the deformation gradient is constant and the liquid crystal director is either aligned uniformly or oriented randomly in Cartesian coordinates. This result generalizes the classical Ericksen’s theorem for nonlinear homogeneous isotropic hyperelastic materials. While Ericksen’s theorem is directly applicable to liquid crystal elastomers in an isotropic phase where the director is oriented randomly, in a nematic phase, the constitutive strain-energy density must account also for the liquid crystal orientation which leads to significant differences in the analysis compared to the purely elastic counterpart.

A theoretical model for power generation via liquid crystal elastomers

Motivated by the need for new materials and green energy production and conversion processes, a class of mathematical models for liquid crystal elastomers (LCEs) integrated within a theoretical charge pump electrical circuit is considered. The charge pump harnesses the chemical and mechanical properties of LCEs transitioning from the nematic to isotropic phase when illuminated or heated to generate higher voltage from a lower voltage supplied by a battery. For the material constitutive model, purely elastic and neoclassical-type strain energy densities applicable to a wide range of monodomain nematic elastomers are combined, while elastic and photothermal responses are decoupled to make the investigation analytically tractable. By varying the model parameters of the elastic and neoclassical terms, it is found that LCEs are more effective than rubber when used as dielectric material within a charge pump capacitor.

Anti-Hertz bulging of actuated liquid crystal elastomers

We consider the ‘anti-Hertz’ elastic problem of inverse indentation, which happens when the surface of an elastic material is pressed down with a plate with a round hole to form a bulge. This classical problem takes on a new life when a polydomain nematic liquid crystal elastomer is used. In this case, the nematic director aligns with the leading principal direction of local stress distribution created by bulging. When the deformed material is crosslinked a second time, this alignment pattern and the resulting permanent protrusion are preserved as pressure is removed, creating a bulge that can be reversibly actuated from a flat surface upon cooling. Experimentally, we also observe a dimple ring around the bulge and a punt (indentation) underneath it at the bottom. Theoretically, we model the deformation by coupling linear elastic and anelastic deformations using non-monotonic nematic elasticity and the singular stress-order relation of the polydomain-monodomain transition. The theory is in excellent agreement with the experiments, and predicts the emergence of all observed features.