Liquid crystalline elastomers: dynamics and relaxation of microstructure (original) (raw)

Anomalous Viscoelastic Response of Nematic Elastomers

Physical Review Letters, 2001

We report a combined theoretical and experimental study of linear viscoelastic response in oriented monodomain nematic elastomers. The model predicts a dramatic decrease in the dynamic modulus in certain deformation geometries in an elastic medium with an independently mobile internal degree of freedom, the nematic director with its own relaxation dynamics. Dynamic mechanical measurements on monodomain nematic elastomers confirm our predictions of dependence on shear geometry and on nematic order, and also show a very substantial mechanical loss clearly associated with director relaxation.

Nonlinear elasticity, fluctuations and heterogeneity of nematic elastomers

Annals of Physics, 2008

Liquid crystal elastomers realize a fascinating new form of soft matter that is a composite of a conventional crosslinked polymer gel (rubber) and a liquid crystal. These solid liquid crystal amalgams, quite similarly to their (conventional, fluid) liquid crystal counterparts, can spontaneously partially break translational and/or orientational symmetries, accompanied by novel soft Goldstone modes. As a consequence, these materials can exhibit unconventional elasticity characterized by symmetry-enforced vanishing of some elastic moduli. Thus, a proper description of such solids requires an essential modification of the classical elasticity theory. In this work, we develop a rotationally invariant, nonlinear theory of elasticity for the nematic phase of ideal liquid crystal elastomers. We show that it is characterized by soft modes, corresponding to a combination of long wavelength shear deformations of the solid network and rotations of the nematic director field. We study thermal fluctuations of these soft modes in the presence of network heterogeneities and show that they lead to a large variety of anomalous elastic properties, such as singular length-scale dependent shear elastic moduli, a divergent elastic constant for splay distortion of the nematic director, long-scale incompressibility, universal Poisson ratios and a nonlinear stress-strain relation for arbitrary small strains. These long-scale elastic properties are universal, controlled by a nontrivial zero-temperature fixed point and constitute a qualitative breakdown of the classical elasticity theory in nematic elastomers. Thus, nematic elastomers realize a stable "critical phase", characterized by universal power-law correlations, akin to a critical point of a continuous phase transition, but extending over an entire phase.

Strain dependence of the nematic fluctuation relaxation in liquid-crystal elastomers

Physical Review E, 2010

Dynamic light scattering on a nematic liquid-crystal elastomer was performed as a function of deformation perpendicular to the director and along the director. We show that the relaxation rate of the nematic director fluctuations increases with strain along the director, as expected from the theory of semisoft elasticity. Deformation applied perpendicular to the director, on the other hand, decreases the relaxation rate to a very small value at the onset of the soft elastic response, revealing the existence of a dynamic soft mode. The results are in complete agreement with the theory of semisoft elasticity and allow us to determine all the constants of the model.

Soft elasticity and mechanical damping in liquid crystalline elastomers

Journal of Applied Physics, 2001

The dynamic soft response of polydomain liquid crystalline elastomers to simple shear is reported. Significantly, these materials also show extremely large loss behavior with tan ␦ exceeding 1 or even 1.5 over very wide temperature ranges, with clear implications for damping applications. By comparing materials that exhibit different types of liquid crystalline phases, we identify the nematic state as a better damping phase than that in materials with smectic phases. Additionally, we provide experimental evidence for directions which should be explored for further improvements in the damping behavior of liquid crystalline elastomers.

Linear hydrodynamics and viscoelasticity of nematic elastomers

European Physical Journal E, 2001

We develop a continuum theory of linear viscoelastic response in oriented monodomain nematic elastomers. The expression for the dissipation function is analogous to the Leslie-Ericksen version of anisotropic nematic viscosity; we propose the relations between the anisotropic rubber moduli and new viscous coefficients. A new dimensionless number is introduced, which describes the relative magnitude of viscous and rubber-elastic torques. In an elastic medium with an independently mobile internal degree of freedom, the nematic director with its own relaxation dynamics, the model shows a dramatic decrease in the dynamic modulus in certain deformation geometries. The degree to which the storage modulus does not altogether drop to zero is shown to be both dependent on frequency and to be proportional to the semi-softness, the non-ideality of a nematic network. We consider the most interesting geometry for the implementation of the theory, calculating the dynamic response to an imposed simple shear and making predictions for effective moduli and (exceptionally high) loss factors.

Internal constraints and arrested relaxation in main-chain nematic elastomers

Nature Communications

Nematic liquid crystal elastomers (N-LCE) exhibit intriguing mechanical properties, such as reversible actuation and soft elasticity, which manifests as a wide plateau of low nearly-constant stress upon stretching. N-LCE also have a characteristically slow stress relaxation, which sometimes prevents their shape recovery. To understand how the inherent nematic order retards and arrests the equilibration, here we examine hysteretic stress-strain characteristics in a series of specifically designed main-chain N-LCE, investigating both macroscopic mechanical properties and the microscopic nematic director distribution under applied strains. The hysteretic features are attributed to the dynamics of thermodynamically unfavoured hairpins, the sharp folds on anisotropic polymer strands, the creation and transition of which are restricted by the nematic order. These findings provide a new avenue for tuning the hysteretic nature of N-LCE at both macro- and microscopic levels via different des...

Viscoelasticity of main chain liquid crystalline elastomers

Polymer, 2006

Time-temperature superposition (TTS) principle was applied to dynamic mechanical analysis performed on two main-chain polydomain elastomers exhibiting a nematic and a smectic A phase. It was found that TTS did not hold neither across the nematic-isotropic nor the smecticisotropic transitions. The nematic elastomer showed an increase in the storage modulus in the isotropic phase with respect to the nematic phase: this could be explained by means of dynamic soft elasticity, which has been claimed in some literature for side-chain liquid crystalline elastomers (SCLCEs), or in terms of the de Gennes model by a macroscopic/hydrodynamic description. The presence of the mesogen directly incorporated into the main chain increases the lifetimes of the elastic modes both in the isotropic and in the liquid crystalline (LC) phases, with respect to the SCLCEs. In the case of the smectic A elastomer, lifetimes on the order of 10 9 s could be estimated. q

Dynamic self-stiffening in liquid crystal elastomers

Nature Communications, 2013

Biological tissues have the remarkable ability to remodel and repair in response to disease, injury, and mechanical stresses. Synthetic materials lack the complexity of biological tissues, and manmade materials which respond to external stresses through a permanent increase in stiffness are uncommon. Here, we report that polydomain nematic liquid crystal elastomers increase in stiffness by up to 90% when subjected to a low-amplitude (5%), repetitive (dynamic) compression. Elastomer stiffening is influenced by liquid crystal content, the presence of a nematic liquid crystal phase and the use of a dynamic as opposed to static deformation. Through rheological and X-ray diffraction measurements, stiffening can be attributed to a nematic director which rotates in response to dynamic compression. Stiffening under dynamic compression has not been previously observed in liquid crystal elastomers and may be useful for the development of self-healing materials or for the development of biocompatible, adaptive materials for tissue replacement.

Nematic fluctuations and semisoft elasticity in swollen liquid-crystal elastomers

Physical review. E, Statistical, nonlinear, and soft matter physics, 2015

Dynamic light scattering (DLS) experiments were performed on stretched sheets of liquid crystal elastomers (LCEs) swollen with a nematic solvent with different swelling ratios. We show that the obtained stress-strain curve and DLS data can still be explained with the concepts of semisoft elasticity. The stress-strain curve shows a typical semisoft response with a threshold strain and a plateau region where stress increases only a little with the applied strain. The width of the plateau decreases with the increase of the swelling ratio because the polymer backbone anisotropy reduces during the swelling. The relaxation rate of thermally excited director fluctuations, however, still shows a typical response, and our measurements indicate the presence of a soft dynamic director-shear mode, as predicted by the theory of semisoft elasticity.

Observation of a Soft Mode of Elastic Instability in Liquid Crystal Elastomers

Physical Review Letters, 2009

In monodomain liquid crystal elastomers a symmetry-breaking locked-in anisotropy causes a semisoft elastic response characterized by a plateau in the stress-strain curve. We show by dynamic light scattering performed as a function of deformation that the relaxation rate of the nematic director fluctuations decreases with strain to a very small value at the onset of the soft elastic response, revealing the existence of a dynamic soft mode. The results are in complete agreement with the theory of semisoft elasticity and allow us to determine all the constants of the model.