Diverse Self-assembly Pathways in Nematic Compartment Network: Topological Percolation and Pathfinding.

The self-assembly of nematic molecules in microcompartments with unambiguously defined surface anchoring is well predictable and is likely to have a single stable topological structure. Here, in contrast, a confined nematic system comprising an array of microcompartments interconnected by channels is demonstrated, exhibiting diverse molecular assembly pathways leading to the formation of four types of topological structures and twelve different patterns randomly distributed. Intercompartment communication via channels plays a crucial role in the diversity of patterns and distributions. It determines the sizes and structures of domains separated by channel defects. The domain structure, which features a pathfinding algorithm and reverse tree structure, can be modelled by an isotropically directed bond percolation with additional restrictions. This system serves as a model for controlled randomness and restricted growth of networks, with potential applications in anticounterfeit protection as a physically unclonable function (PUF) with multiple-level communication protocols.

Response to an applied electric field in an antiferroelectric 1/2 subphase: The role of thermal fluctuations.

The response to an applied electric field in the q_{T}=1/2 subphase of the MC881-MC452 binary mixture system is studied by using thick homeotropically aligned cells. In the ordinary antiferroelectric SmC_{A}^{*} and 1/2 (sub)phases, some nonplanar asymmetric distortions in the antiferroelectric unit cell structure produce induced polarization in the applied field direction, starts to unwind the helix from the beginning, and tends to align the averaged tilt plane direction parallel to the applied field. In the 1/2 subphase under consideration, however, the helix resists being deformed at the beginning and then the thresholdlike steep increase of birefringence Δn occurs in the transition from 1/2 to unwound SmC^{*} at a field of less than 0.5 V/µm; we conclude that the thermal fluctuations play an important role in promoting the director flip-flopping in a single layer under the applied field and bring about additional induced polarization, which counteracts the aforementioned ordinary induced one and prevents the helix from unwinding. This suggests that the Langevin-like director reorientation is the mechanism of the V-shaped switching which was actually observed in the thin films of Mitsui mixture [Phys. Rev. Lett. 87, 015701 (2001)0031-900710.1103/PhysRevLett.87.015701] and must have been used in prototyped thresholdless antiferroelectric liquid-crystal displays.

Rotation-Time Symmetry Breaking in Frustrated Chiral Nematic Driven by a Pulse-Train Waveform.

We report waveform-induced rotation-time symmetry breaking in liquid crystal director motion. Homeotropic cells filled with a negative dielectric anisotropy chiral nematic exhibit persistent and visually observable waves of director orientation with a time period of at least 30 driving field cycles. Their existence in the space of driving waveform parameters is explored. The possibility of utilizing this system, which exhibits both spatial and temporal long-range order, as a modeling tool for experimental studies on discrete time crystals is discussed.

Dielectric study of a subphase stabilized in an exceptionally wide temperature range by a delicate balance of interlayer interactions and thermal fluctuations.

The chiral smectic phases of calamitic liquid crystals, SmC^{*} and SmC_{A}^{*}, are characterized by the synclinic ferroelectric F ordering and the anticlinic antiferroelectric A ordering in adjacent layers. Various states with mixed A and F orderings are degenerate at the frustrated phase-transition point. The degeneracy lifting is commonly caused by the long-range interlayer interactions (LRILIs), producing a series of biaxial subphases specified by a relative ratio of both orderings, q_{T}=[F]/([A]+[F]). Sandhya et al. [Phys. Rev. E 87, 012502 (2013)PLEEE81539-375510.1103/PhysRevE.87.012502] established, however, the importance of thermal fluctuations in the degeneracy lifting in some binary mixtures of MC881 and MC452. They observed the most intriguing interplay of thermal fluctuations and LRILIs in the stabilization of an apparently single subphase. Since no other detailed experimental study of the subphase has so far been made, we carry out its dielectric investigations and clarify the following five points: (1) the subphase is surely a single phase from ≈80^{∘}C down to room temperature; (2) the imaginary part of complex permittivity ε^{″} shows the weak antiphase mode and hence it must be antiferroelectric q_{T}=1/2; (3) ε^{″} becomes much stronger above ≈80^{∘}C, indicating the emergence of ferroelectric and/or ferrielectric states; (4) the dielectric amplitude gradually increases at least just above the 1/2 subphase, suggesting it be due to a continuous increase of q_{T}; and (5) at low temperatures the antiphase relaxation mode shows irregularities that indicate the important role played by the cooperative motion of the layer undulation as well as of the director tilting.

Characterization of the Submicrometer Hierarchy Levels in the Twist-Bend Nematic Phase with Nanometric Helices via Photopolymerization. Explanation for the Sign Reversal in the Polar Response.

Photopolymerization of a reactive mesogen mixed with a mesogenic dimer, shown to exhibit the twist-bend nematic phase (NTB), reveals the complex structure of the self-deformation patterns observed in planar cells. The polymerized reactive mesogen retains the structure formed by liquid crystalline molecules in the twist bend phase, thus enabling its observation by scanning electron microscopy (SEM). Hierarchical ordering scales ranging from tens of nanometers to micrometers are imaged in detail. Submicron features, anticipated from earlier X-ray experiments, are visualized directly. In the self-deformation stripes formed in the NTB phase, the average director field is found tilted in the cell plane by an angle of up to 45° from the cell rubbing direction. This tilt explains the sign inversion being observed in the electro-optical studies.

Spontaneous helix formation in non-chiral bent-core liquid crystals with fast linear electro-optic effect.

Liquid crystals (LCs) represent one of the foundations of modern communication and photonic technologies. Present display technologies are based mainly on nematic LCs, which suffer from limited response time for use in active colour sequential displays and limited image grey scale. Herein we report the first observation of a spontaneously formed helix in a polar tilted smectic LC phase (SmC phase) of achiral bent-core (BC) molecules with the axis of helix lying parallel to the layer normal and a pitch much shorter than the optical wavelength. This new phase shows fast (∼30 µs) grey-scale switching due to the deformation of the helix by the electric field. Even more importantly, defect-free alignment is easily achieved for the first time for a BC mesogen, thus providing potential use in large-scale devices with fast linear and thresholdless electro-optical response.

Short-range correlations seen in the nematic phase of bent-core liquid crystals by dielectric and electro-optic studies.

Three bent-core nematic liquid crystals having the same core but with different terminal groups, short (C4) and long (C7,C9) tails, are investigated by dielectric and electro-optic contrast spectroscopic techniques. C4 shows sign reversal in the dielectric anisotropy Δε' as a function of both temperature and frequency, whereas C9 shows only negative Δε' in the entire mesophasic region. The behavior of C7 is intermediate of the two. Results of a dielectric study show that both C7 and C9 exhibit strong short-range polar correlations normal to the director. The correlation lengths of these interactions are found to be similar to those from the x-ray scattering. An increased hindered rotation for C9 compared to C4 moves the dielectric dispersion for ε(|') to much lower frequencies, such that C9 shows only negative Δε' over the entire temperature range.

Orientational order of a ferroelectric liquid crystal with small layer contraction.

We present spectroscopic and optical studies of a non-layer-shrinkage ferroelectric liquid crystal DSiKN65. The orientational order parameters S, measured with respect to the smectic layer normal using IR spectroscopy on a sample aligned homeotropically, does not exhibit any significant variation between the smectic-A∗ and smectic-C∗ phases. In contrast the birefringence of a planar homogenous sample abruptly increases at the smectic-A∗ to smectic-C∗ transition. This suggests a general increase in the orientational order, which can be described by the orientational order parameters S' defined with respect to the director. Simultaneous increase of S' and the director tilt Θ may explain the low shrinkage of smectic layers, which is consistent with recent theoretical models describing the smectic-A∗ to smectic-C∗ transition for such materials.