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See detailTowards tunable defect arrangements in smectic liquid crystal shells utilizing the nematic-smectic transition in hybrid-aligned geometries
Liang, Hsin-Ling; Zentel, Rudolf; Rudquist, Per et al

in Soft Matter (2012), 8(20), 5443-5450

We produce and investigate liquid crystal shells with hybrid alignment—planar at one boundary, homeotropic at the other—undergoing a transition between the nematic (N) and smectic-A (SmA) phases. The ... [more ▼]

We produce and investigate liquid crystal shells with hybrid alignment—planar at one boundary, homeotropic at the other—undergoing a transition between the nematic (N) and smectic-A (SmA) phases. The shells display a dynamic sequence of patterns, the details depending on the alignment agents and on the diameter and thickness of the shell. In shells of sufficient diameter we typically find a transient striped texture near the N–SmA transition, stabilising into a pattern of tiled, more or less regularly spaced focal conic domains in the SmA phase. The domain size and spacing decrease with reduced shell thickness. In case of strong homeotropic anchoring at one boundary and small shell size, however, the increased curvature favors homeotropic against planar alignment in the smectic phase, and the shell then tends to adapt to complete homeotropic alignment at the final stage of the transition. This is the first study of hybrid-aligned smectic shells and the results constitute a beautiful demonstration of the capacity for dynamic structure formation and reformation via self-assembly in soft matter. The new patterns extend the range of arrays of topological defects that can be realised with liquid crystals in spherical morphology and the correlation between the feature arrangements and the variable parameters of the shell and its environment opens a route towards tunability. However, the observed strong impact from increasing curvature, even for these rather large shells, indicates that the choice of alignment agents inducing planar or homeotropic alignment with varying strength will become critical when targeting the most attractive colloidal size scale of about a micron or smaller. [less ▲]

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See detailNematic-smectic transition under confinement in liquid crystalline colloidal shells
Liang, Hsin-Ling; Schymura, Stefan; Rudquist, Per et al

in Physical Review Letters (2011), 106(24), 247801

We carry out the first study of smectic liquid crystalline colloidal shells and investigate how their complex internal structure depends on the director configuration in the nematic phase, preceding the ... [more ▼]

We carry out the first study of smectic liquid crystalline colloidal shells and investigate how their complex internal structure depends on the director configuration in the nematic phase, preceding the smectic phase on cooling. Differences in the free energy cost of director bend and splay give an initial skewed distribution of topological defects in the nematic phase. In the smectic phase, the topological and geometrical constraints of the spherical shell imposed on the developing 1D quasi-long-range order create a conflict that triggers a series of buckling instabilities. Two different characteristic defect patterns arise, one driven by the curvature of the shell, the other by the strong nonuniformities in the director field in the vicinity of the topological defects. [less ▲]

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See detailChiral smectic C subphases induced by mixing a bistereogenic antiferroelectric liquid crystal with a non-chiral liquid crystal
Lagerwall, Jan UL; Giesselmann, Frank; Rauch, Sebastian et al

in Ferroelectrics (2005), 315

By mixing a bistereogenic antiferroelectric liquid crystal (AFLC) compound, exhibiting only the SmQ and SmCa mesophases, with the achiral N-SmC liquid crystal HOAB we could induce all three AFLC SmC-type ... [more ▼]

By mixing a bistereogenic antiferroelectric liquid crystal (AFLC) compound, exhibiting only the SmQ and SmCa mesophases, with the achiral N-SmC liquid crystal HOAB we could induce all three AFLC SmC-type subphases, SmCalpha, SmCbeta and SmCgamma. This seems to be in contradiction with two recent postulations regarding the subphase stability, one of which suggests that the subphases appear as a result of strong chiral interactions, the other that these phases require high smectic order something one would generally not expect in mixtures. We have studied the helical pitch, optical tilt angle, spontaneous polarization and the x-ray diffraction due to the smectic layering, as a function of mixing ratio in order to better understand the relation between phase sequence and mixture composition. The smectic layer spacing shows a strongly non-linear behavior suggesting that the basic structure of the pure AFLC substance is retained up to a HOAB content of about 75\%. [less ▲]

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See detailOn the phase sequence of antiferroelectric liquid crystals and its relation to orientational and translational order
Lagerwall, Jan UL; Rudquist, Per; Lagerwall, Sven T. et al

in Liquid Crystals (2003), 30(4), 399-414

The substance MHPOBC is the oldest and still most important reference antiferroelectric liquid crystal (AFLC). There is still considerable controversy concerning the correct phase designations for this ... [more ▼]

The substance MHPOBC is the oldest and still most important reference antiferroelectric liquid crystal (AFLC). There is still considerable controversy concerning the correct phase designations for this material and, in particular, about the presence or absence of SmC* in its phase sequence. By means of dielectric spectroscopy and polarizing microscopy, we show that whereas the pure compound lacks the SmC* phase, this phase rapidly replaces the SmC*b subphase through the reduced purity resulting from temperature-induced chemical degradation which is hard to avoid under standard experimental conditions. X-ray investi- gations furthermore show that this change in phase sequence is coupled to a decrease in translational order. This explains the large variations in the reported phase sequence and electro-optic behaviour of MHPOBC, in particular concerning the SmC*b phase which has been said to exhibit ferro-, ferri- as well as antiferroelectric properties. It is likely that the sensitivity of the AFLC phase sequence to sample purity is a general property of AFLC materials. We discuss the importance of optical and chemical purity as well as tilt and spontaneous polarization for the observed phase sequence and propose that one of the key features determining the existence of the different tilted structures is the antagonism between orientational (nematic) and translational (smectic) order. The decreased smectic order (increased layer interdigitation) imposed by chemical impurities promotes the synclinic SmC* phase at the cost of the AFLC phases SmC*a , SmC*b , SmC*c and SmC*a . We also propose that the SmA* phase in FLC and AFLC materials may actually have a somewhat different character and, depending on its microstructure, some of the tilted phases can be expected to appear or not to appear in the phase sequence. AFLC materials exhibiting a direct SmA*–SmC*a transition are found to be typical ‘de Vries smectics’, with very high orientational disorder in the SmA* phase. Finally, we discuss the fact that SmC*b and SmC*c have two superposed helical superstructures and explain the observation that the handedness of the large scale helix may very well change sign, while the handedness on the unit cell level is preserved. [less ▲]

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See detailSurface- and field-induced AFLC structures detected by dielectric spectroscopy
Lagerwall, Jan UL; Rudquist, Per; Lagerwall, Sven T. et al

in Ferroelectrics (2002)

In order to better understand which features in dielectric spectra of antiferroelectric liquid crystals (AFLCs) are due to the bulk director geometry and which are due to surface-induced structures, we ... [more ▼]

In order to better understand which features in dielectric spectra of antiferroelectric liquid crystals (AFLCs) are due to the bulk director geometry and which are due to surface-induced structures, we have performed dielectric spectroscopy measurements with simultaneous texture monitoring on two SmC*-exhibiting AFLC homologues (11- and 12F1M7), at varying cell gap. Such AFLCs are strongly affected by surface action even in fairly thick cells (d≈15µm), with heavy supercooling of the SmC* phase as the most obvious result. We show that the supercooled structure can be removed by AC-field treatment in the SmCa* phase, but some domains may stay in a polar geometry, as reflected in both texture and dielectric signature. On heating from the antiferroelectric SmC?* subphase into SmC*, meta-stable non-helical domains may form at cell gaps much larger than the helical pitch. These domains give rise to a lowfrequency dielectric absorption not seen in bulk SmC* samples. [less ▲]

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See detailTilt plane orientation in antiferroelectric liquid crystal cells and the origin of the pretransitional effect
Rudquist, Per; Lagerwall, Jan UL; Meier, Johann G. et al

in Physical Review. E : Statistical, Nonlinear, and Soft Matter Physics (2002), 66(6), 061708

The optic, electro-optic, and dielectric properties of antiferroelectric liquid crystals 􏰐AFLCs􏰋 are analyzed and discussed in terms of the local tilt plane orientation. We show that the so-called ... [more ▼]

The optic, electro-optic, and dielectric properties of antiferroelectric liquid crystals 􏰐AFLCs􏰋 are analyzed and discussed in terms of the local tilt plane orientation. We show that the so-called pretransitional effect is a combination of two different electro-optic modes: the field-induced antiphase distortion of the antiferroelectric structure and the field-induced reorientation of the tilt plane. In the presence of a helix, the latter corresponds to a field-induced distortion of the helix. Both electro-optic modes are active only when the electric field has a component along the tilt plane. Thus, by assuring a horizontal surface-stabilized condition, where the helix is unwound by surface action and the tilt plane is everywhere parallel to the cell plates, the pretransitional effect should be suppressed. We also discuss the dielectrically active modes in AFLCs and under which circum- stances they contribute to the measured dielectric permittivity. [less ▲]

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See detailAntiferroelectric liquid crystals with 45° tilt - a new class of promising electro-optic materials
D’havé, K.; Dahlgren, A; Rudquist, Per et al

in Ferroelectrics (2000), 244

Antiferroelectric liquid crystals with a tilt angle of 45 degrees have very interesting optical properties, which seem to have been overlooked so far perhaps because such materials have hardly been ... [more ▼]

Antiferroelectric liquid crystals with a tilt angle of 45 degrees have very interesting optical properties, which seem to have been overlooked so far perhaps because such materials have hardly been available. We have prepared a four-component mixture of partially fluorinated compounds with a SmC/sub n/* phase in the interval between 27.4 degrees C and 121.6 degrees C, in which the tilt angle theta saturates at 45 degrees for T<or=80 degrees C, and we investigate the optical properties, theoretically and experimentally. One of the surprising features of 45 degree materials is that they permit a remarkably high contrast by virtue of an excellent dark-state, in spite of the fact that AFLC materials are notoriously difficult to align. This is because a 45 degrees AFLC turns out to be (negatively) uniaxial instead of biaxial. We describe these properties and propose a number of potentially interesting new applications, including a polarizer-free display mode and a three-level ``phase-only'' modulator. [less ▲]

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See detailThe case of thresholdless antiferroelectricity: Polarization-stabilized twisted SmC* liquid crystals give V-shaped electro-optic response
Rudquist, Per; Lagerwall, Jan UL; Buivydas, M. et al

in Journal of Materials Chemistry (1999), 9(6), 1257-1261

We have studied the three-component liquid crystal mixture reported to exhibit ‘thresholdless antiferroelectricity’ [Inui et al., J. Mater. Chem, 1996, 6, 671]. We find that the thresholdless or V-shaped ... [more ▼]

We have studied the three-component liquid crystal mixture reported to exhibit ‘thresholdless antiferroelectricity’ [Inui et al., J. Mater. Chem, 1996, 6, 671]. We find that the thresholdless or V-shaped switching is obtained in thf absence of antiferroelectricity. This analog electro-optic response is due to the field-induced switching of a twisted smectic C* structure stabilized by polar surface interactions and by electrostatic bulk polarization charge interactions. The latter confine the director twist to thin surface regions leaving the bulk of the cell uniform, which gives good extinction at zero field. In sufficiently thin cells, such thresholdless switching can in fact be followed down to much lower temperatures, where the bulk would be antiferroelectric, but is maintained in the cells in the ferroelectric state by hysteresis from surface action. [less ▲]

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