Stenull and Lubensky [Phys. Rev. E {\bf 76}, 011706 (2007)] have argued that shear strain and tilt of the director relative to the layer normal are coupled in smectic elastomers and that the imposition of one necessarily leads to the development of the other. This means, in particular, that a Smectic-A elastomer subjected to a simple shear will develop Smectic-C-like tilt of the director. Recently, Kramer and Finkelmann [arXiv:0708.2024, Phys. Rev. E {\bf 78}, 021704 (2008)] performed shear experiments on Smectic-A elastomers using two different shear geometries. One of the experiments, which implements simple shear, produces clear evidence for the development of Smectic-C-like tilt. Here, we generalize a model for smectic elastomers introduced by Adams and Warner [Phys. Rev. E {\bf 71}, 021708 (2005)] and use it to study the magnitude of Smectic-C-like tilt under shear for the two geometries investigated by Kramer and Finkelmann. Using reasonable estimates of model parameters, we estimate the tilt angle for both geometries, and we compare our estimates to the experimental results. The other shear geometry is problematic since it introduces additional in-plane compressions in a sheet-like sample, thus inducing instabilities that we discuss.
Smectic-C elastomers can be prepared by crosslinking, e.g., liquid crystal polymers, in the smectic-A phase followed by a cooling through the smectic-A to smectic-C phase transition. This transition from $D_{\infty h}$ to $C_{2h}$ symmetry spontaneously breaks rotational symmetry in the smectic plane as does the transition from a smectic-A to a biaxial smectic phase with $D_{2h}$ symmetry. We study these transitions and the emergent elasticity of the smectic-C and biaxial phases in three related models and show that these phases exhibit soft elasticity analogous to that of nematic elastomers.
We present a model for smectic elastomer membranes which includes elastic and liquid crystalline degrees of freedom. Based on our model, we determined the qualitative phase diagram of a smectic elastomer membrane using mean-field theory. This phase diagram is found to comprise five phases, viz. smectic-A--flat, smectic-A--crumpled, smectic-C--flat, smectic-C--crumpled and smectic-C--tubule, where in the latter phase, the membrane is flat in the direction of mesogenic tilt and crumpled in the perpendicular direction. The transitions between adjacent phases are second order phase transitions. We…
We study two aspects of the elasticity of smectic-$A$ elastomers that make these materials genuinely and qualitatively different from conventional uniaxial rubbers. Under strain applied parallel to the layer normal, monodomain smectic-$A$ elastomers exhibit a drastic change in Young's modulus above a threshold strain value of about 3%, as has been measured in experiments by Nishikawa and Finkelmann [Macromol. Chem. Phys. {\bf 200}, 312 (1999)]. Our theory predicts that such strains induce a transition to a smectic-$C$-like state and that it is this transition that causes the change in elastic …
We present a detailed analysis of the molecular packing of a strained liquid crystal elastomer composed of chiral mesogens in the smectic A phase. X-ray diffraction patterns of the elastomer collected over a range of orientations with respect to the X-ray beam were used to reconstruct the three-dimensional scattering intensity as a function of tensile strain. For the first time, we show that the smectic domain order is preserved in these strained elastomers. Changes in the intensity within a given scattering plane are due to reorientation, and not loss, of the molecular order in directions ort…
Models of smectic-C liquid crystal elastomers predict that it can display soft elasticity, in which the shape of the elastomer changes at no energy cost. The amplitude of the soft mode and the accompanying shears are dependent on the orientation of the layer normal and the director with respect to the stretch axis. We demonstrate that in some geometries the director is forced to rotate perpendicular to the stretch axis, causing lateral expansion of the sample; a negative Poisson's ratio. Current models do not include the effect of imperfections that must be present in the physical sample. We i…
We study anomalous elasticity in the tubule phases of nematic and smectic elastomer membranes, which are flat in one direction and crumpled in another. These phases share the same macroscopic symmetry properties including spontaneously-broken in-plane isotropy and hence belong to the same universality class. Below an upper critical value $D_c =3$ of the membranes' intrinsic dimension D, thermal fluctuations renormalize the elasticity with respect to elastic displacements along the tubule axis so that elastic moduli for compression along the tubule axis and for bending the tubule axis become le…
Elastomers are artificial polymeric materials created for industrial and commercial applications. Depending on their purpose, they are performing in different species and structure modifications. Our studies focus on the systems of elastomers randomly standing-distributed in a smectic $A$ (Sm$A$) liquid crystal. Basing on the suggestion following from the experiment, that at a phase transition from Sm$A$ to nematic phase caused by an increase of a crosslink concentration, such a system survives a percolation transition at low crossilink concentrations, we propose a modeling explaining this phe…
We present a numerical study of stretching monodomain smectic-A elastomer sheets, computed using the finite element method. When stretched parallel to the layer normal the microscopic layers in smectic elastomers are unstable to a transition to a buckled state. We account for the layer buckling by replacing the microscopic energy with a coarse grained effective free energy that accounts for the fine scale deformation of the layers. We augment this model with a term to describe the energy of deforming buckled layers, which is necessary to reproduce the experimentally observed Poisson's ratios p…
We present a theory for the low-frequency, long-wavelength dynamics of soft smectic-C elastomers with locked-in smectic layers. Our theory, which goes beyond pure hydrodynamics, predicts a dynamic soft elasticity of these elastomers and allows us to calculate the storage and loss moduli relevant for rheology experiments as well as the mode structure.
We study the low-frequency, long-wavelength dynamics of liquid crystal elastomers, crosslinked in the smectic-$A$ phase, in their smectic-$A$, biaxial smectic and smectic-$C$ phases. Two different yet related formulations are employed. One formulation describes the pure hydrodynamics and does not explicitly involve the Frank director, which relaxes to its local equilibrium value in a non-hydrodynamic time. The other formulation explicitly treats the director and applies beyond the hydrodynamic limit. We compare the low-frequency, long-wavelength dynamics of smectic-$A$ elastomers to that of ne…
The reorientation behaviour of a smectic-A (SmA) elastomer deformed parallel to the smectic layer normal has been interpreted as a Sm-C like transition by Stenull and Lubensky. Experiments, however, prove that such a transition does not occur.
Ideal (monodomain) smectic-$A$ elastomers crosslinked in the smectic-$A$ phase are simply uniaxial rubbers, provided deformations are small. From these materials smectic-$C$ elastomers are produced by a cooling through the smectic-$A$ to smectic-$C$ phase transition. At least in principle, biaxial smectic elastomers could also be produced via cooling from the smectic-$A$ to a biaxial smectic phase. These phase transitions, respectively from $D_{\infty h}$ to $C_{2h}$ and from $D_{\infty h}$ to $D_{2h}$ symmetry, spontaneously break the rotational symmetry in the smectic planes. We study the ab…
Experimentally it is possible to manipulate the director in a (chiral) smectic-$A$ elastomer using an electric field. This suggests that the director is not necessarily locked to the layer normal, as described in earlier papers that extended rubber elasticity theory to smectics. Here, we consider the case that the director is weakly anchored to the layer normal assuming that there is a free energy penalty associated with relative tilt between the two. We use a recently developed weak-anchoring generalization of rubber elastic approaches to smectic elastomers and study shearing in the plane of …
Structural studies by synchrotron x-ray diffraction on two main-chain smectic-C elastomers reveal the presence of two different relaxation mechanisms in these systems at low and high strains. At low strains, the smectic layers are reoriented with layer-normals distributed in a plane perpendicular to the stretch direction. The system relaxes relatively slowly (time-constant ~ 45 minutes) which is attributed to the flow properties of the LC layers embedded in the elastomer network. At high strains, the equilibration time (~ 4 - 8 minutes) conforms to a faster relaxation and appears to have its o…
On the emergence of molecular tilt in a ferroelectric smectic liquid crystal with broken director-inversion symmetry
University of the Basque Country EHU（巴斯克大学）；Universidad de Zaragoza（萨拉戈萨大学）；Instituto de Nanociencia y Materiales de Aragón (INMA), CSIC-Universidad de Zaragoza（阿拉贡纳米科学与材料研究所（INMA），西班牙国家研究委员会-萨拉戈萨大学）；Universitat Politècnica de Catalunya（加泰罗尼亚理工大学）
We present and analyze a model for the combination of bulk and surface electroclinic effects in the smectic-A* (Sm-A) phase near a Sm-A*--Sm-C* transition. As part of our analysis we calculate the dependence of the surface tilt on external electric field and show that it can be eliminated, or even reversed from its zero-field value. This is in good agreement with previous experimental work on a system (W415) with a continuous Sm-A*--Sm-C* transition. We also analyze, for the first time, the combination of bulk and surface electroclinic effects in systems with a first order Sm-A*--Sm-C* transit…
We analyze the surface electroclinic effect (SECE) in a material that exhibits a first order bulk smectic-$A^*$ (Sm-$A^*$) -- smectic-$C^*$ (Sm-$C^*$) transition. The effect of a continuously varying degree of enantiomeric excess on the SECE is also investigated. We show that due to the first order nature of the bulk Sm-$A^*$ -- Sm-$C^*$ transition, the SECE can be unusually strong and that as enantiomeric excess is varied, a jump in surface induced tilt is expected. A theoretical state map, in enantiomeric excess - temperature space, features a critical point which terminates a line of first …
Using a generalized Landau theory involving orientational, layering, tilt, and biaxial order parameters we analyze the smectic-A* and smectic-C* (Sm-A* -- Sm-C*) transition, showing that a combination of small orientational order and large layering order leads to Sm-A* -- Sm-C* transitions that are either continuous and close to tricriticality or first order. The model predicts that in such systems the increase in birefringence upon entry to the Sm-C* phase will be especially rapid. It also predicts that the change in layer spacing at the Sm-A* -- Sm-C* transition will be proportional to the o…
The order parameters for the phenomenological description of the smectic-{\it A} to smectic-{\it C} phase transition are formulated on the basis of molecular symmetry and structure. It is shown that, unless the long molecular axis is an axis of two-fold or higher rotational symmetry, the ordering of the molecules in the smectic-{\it C} phase gives rise to more than one tilt order parameter and to one or more polar order parameters. The latter describe the indigenous polarity of the smectic-{\it C} phase, which is not related to molecular chirality but underlies the appearance of spontaneous po…
Chiral liquid crystals often exhibit periodic modulations in the molecular director; in particular, thin films of the smectic-C* phase show a chiral striped texture. Here, we investigate whether similar chiral modulations can occur in the induced molecular tilt of the smectic-A phase under an applied electric field. Using both continuum elastic theory and lattice simulations, we find that the state of uniform induced tilt can become unstable when the system approaches the smectic-A--smectic-C* transition, or when a high electric field is applied. Beyond that instability point, the system devel…
The phase behavior of the system of parallel rigid triblock copolymers is examined using the second-virial density functional theory. The triblock particle consists of two identical infinitely thin hard rods of finite lengths on the opposite ends of one central hard cylinder with nonzero length and diameter. Stability analyses and free energy calculations show that the system of parallel particles can form not only uniform nematic and smectic A phases, but a smectic-C phase too. The stability and structure of the tilted structure is controlled by only the diameter and the length of the central…
An unresolved issue in the theory of liquid crystals is the molecular basis of the electroclinic effect in the smectic-A phase. Recent x-ray scattering experiments suggest that, in a class of siloxane-containing liquid crystals, an electric field changes a state of disordered molecular tilt in random directions into a state of ordered tilt in one direction. To investigate this issue, we measure the optical tilt and birefringence of these liquid crystals as functions of field and temperature, and we develop a theory for the distribution of molecular orientations under a field. Comparison of the…
Using Monte Carlo simulation methods, we explore the role of molecular shape in the phase behavior of liquid crystals and the electroclinic effect. We study a "bent-rod" mesogen shaped like the letter Z, composed of seven soft spheres bonded rigidly together with no intra-molecular degrees of freedom. For strongly angled molecules, we find that steric repulsion alone provides the driving force for a smectic-C phase, even without intermolecular dipole-dipole interactions. For weakly angled (nearly rod-like) molecules, we find a stable smectic-A (SmA) phase and a strong electroclinic effect with…
