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Register a new userStructures and orientational transitions in thin films of tilted hexatic smectics
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We present detailed systematic studies of structural transformations in thin liquid crystal films with the smectic-C to hexatic phase transition. For the first time all possible structures reported in the literature are observed for one material (5 O.6) at the variation of temperature and thickness. In unusual modulated structures the equilibrium period of stripes is twice with respect to the domain size. We interpret these patterns in the frame work of phenomenological Landau type theory, as equilibrium phenomena produced by a natural geometric frustration in a system having spontaneous splay distortion.
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The Landau theory of phase transitions has been productively applied to phase transitions that involve rotational symmetry breaking, such as the transition from an isotropic fluid to a nematic liquid crystal. It even can be applied to the orientational symmetry breaking of simple atomic or molecular clusters that are not true phase transitions. In this paper we address fundamental problems that arise with the Landau theory when it is applied to rotational symmetry breaking transitions of more complex particle clusters that involve order parameters characterized by larger values of the $l$ index of the dominant spherical harmonic that describes the broken symmetry state. The problems are twofold. First, one may encounter a thermodynamic instability of the expected ground state with respect to states with lower symmetry. A second problem concerns the proliferation of quartic invariants that may or may not be physical. We show that the combination of a geometrical method based on the analysis of the space of invariants, developed by Kim to study symmetry breaking of the Higgs potential, with modern visualization tools provides a resolution to these problems. The approach is applied to the outcome of numerical simulations of particle ordering on a spherical surface and to the ordering of protein shells.
We report on X-ray studies of freely suspended hexatic films of three different liquid crystal compounds. By applying angular X-ray cross-correlation analysis (XCCA) to the measured diffraction patterns the parameters of the bond-orientational (BO) order in the hexatic phase were directly determined. The temperature evolution of the BO order parameters was analyzed on the basis of the multicritical scaling theory (MCST). Our results confirmed the validity of the MCST in the whole temperature range of existence of the hexatic phase for all three compounds. The temperature dependence of the BO order parameters in the vicinity of the hexatic-smectic transition was fitted by a conventional power law with a critical exponent $betaapprox0.1$ of extremely small value. We found that the temperature dependence of higher order harmonics of the BO order scales as the powers of the first harmonic, with exponent equal to harmonic number. This indicates a nonlinear coupling of the BO order parameters of different order. It is shown that compounds of various composition, possessing different phase sequences, display the same thermodynamic behavior in the hexatic phase and in the vicinity of the smectic-hexatic phase transition.
We investigate the relaxation behavior of thin films of a polyamide random copolymer, PA66/6I, with various film thicknesses using dielectric relaxation spectroscopy. Two dielectric signals are observed at high temperatures, the $alpha$-process and the relaxation process due to electrode polarization (the EP-process). The relaxation time of the EP-process has a Vogel-Fulcher-Tammann type of temperature dependence, and the glass transition temperature, $T_{rm g}$, evaluated from the EP-process agrees very well with the $T_{rm g}$ determined from the thermal measurements. The fragility index derived from the EP-process increases with decreasing film thickness. The relaxation time and the dielectric relaxation strength of the EP-process are described by a linear function of the film thickness $d$ for large values of $d$, which can be regarded as experimental evidence for the validity of attributing the observed signal to the EP-process. Furthermore, there is distinct deviation from this linear law for thicknesses smaller than a critical value. This deviation observed in thinner films is associated with an increase in the mobility and/or diffusion constant of the charge carriers responsible for the EP-process. The $alpha$-process is located in a high frequency region than the EP-process at high temperatures, but merges with the EP-process at lower temperatures near the glass transition region. The thickness dependence of the relaxation time of the $alpha$-process is different from that of the EP-process. This suggests that there is decoupling between the segmental motion of the polymers and the translational motion of the charge carriers in confinement.
Coarse-grained molecular-dynamics simulations were used to study the morphological changes induced in a Nafion$^{tiny textregistered}$-like ionomer by the imposition of a strong electric field. We observe the formation of novel structures aligned along the direction of the applied field. The polar head groups of the ionomer side chains aggregate into clusters, which then form rod-like formations which assemble into a hexatic array aligned with the direction of the field. Occasionally these lines of sulfonates and protons form a helical structure. Upon removal of the electric field, the hexatic array of rod-like structures persists, and has a lower calculated free energy than the original isotropic morphology.
Structure of polymer electrolytes membranes, e.g., Nafion, inside fuel cell catalyst layers has significant impact on the electrochemical activity and transport phenomena that determine cell performance. In those regions, Nafion can be found as an ultra-thin film, coating the catalyst and the catalyst support surfaces. The impact of the hydrophilic/hydrophobic character of these surfaces on the structural formation of the films and, in turn, on transport properties, has not been sufficiently explored yet. Here, we report about classical Molecular Dynamics simulations of hydrated Nafion thin-films in contact with unstructured supports, characterized by their global wetting properties only. We have investigated structure and transport in different regions of the film and found evidences of strongly heterogeneous behavior. We speculate about the implications of our work on experimental and technological activity.
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