arXiv subjects

Lech Longa

Publications and source records attributed to Lech Longa.

16 recordsLinked to original sources

arXiv2025

Confinement Reveals Hidden Splay-Bend Order in Twist-Bend Nematics

Using extensive Monte Carlo (MC) and molecular dynamics (MD) simulations, we investigate how spatial confinement affects molecular organization within thin films of the nematic twist-bend ($\mathrm{N_{TB}}$) phase. Our simulations show that confinement markedly amplifies the otherwise elusive splay-bend order, primarily by suppressing the intrinsic three-dimensional heliconical structure characteristic of bulk $\mathrm{N_{TB}}$. Remarkably, when the $\mathrm{N_{TB}}$ phase is confined between parallel walls imposing planar anchoring, and the bulk wave vector is oriented parallel to the walls, a smectic splay-bend ($\mathrm{S_{SB}}$) phase spontaneously emerges near the confining surfaces. This intermediate structure subsequently transforms into the bulk $\mathrm{N_{TB}}$ phase either directly via a smectic splay-bend-twist ($\mathrm{S_{SBT}}$) phase or through a sequence involving both the $\mathrm{S_{SBT}}$ and the nematic splay-bend-twist ($\mathrm{N_{SBT}}$) phases. Notably, the $\mathrm{N_{SBT}}$ phase becomes particularly pronounced as the molecular bend angle approaches its maximum attainable value in bulk $\mathrm{N_{TB}}$; this regime occurs in close proximity to the $\mathrm{N}\text{--}\mathrm{S_{A}}\text{--}\mathrm{S_{SB}}$ triple point on the bulk phase diagram. Our findings reveal a compelling and intricate interplay among chirality, confinement, and molecular ordering, further evidenced by the calculated elementary director distortions. Crucially, this study opens promising avenues for experimental exploration: confined thin-film geometries serve as powerful model systems for revealing and characterizing novel nematic and smectic liquid-crystal phases that remain elusive in, or currently inaccessible to, bulk experiments.

cond-mat.soft↗

arXiv2024

Ferroelectric nematic phase in the system of perfectly aligned cyllindrically symmetric rods

The recent experimental discovery of ferroelectric and splay nematic phases has sparked interest in comprehending the crucial molecular features necessary to stabilize these innovative structures. This study advances the ongoing discourse by investigating the significance of both molecular elongation and the distribution of molecular dipoles along the main molecular axis. Using Density Functional Theory, we have established that a molecular shape characterized by cylindrical symmetry and the presence of strong parallel dipoles along the symmetry axis can lead to the self-assembly of a ferroelectric nematic, which is more stable than the conventional uniaxial nematic phase. Additionally, we provide criteria for achieving an optimal dipole distribution along the molecular axis.

cond-mat.soft↗

arXiv2022

Conformational degrees of freedom and stability of splay-bend ordering in the limit of a very strong planar anchoring

We study the self-organization of flexible planar trimer particles on a structureless surface. The molecules are made up of two mesogenic units linked by a spacer, all of which are modeled as hard needles of the same length. Each molecule can dynamically adopt two conformational states: an achiral bent-shaped (cis-) and a chiral zigzag (trans-) one. Using constant pressure Monte Carlo simulations and Onsager-type density functional theory (DFT), we show that the system consisting of these molecules exhibits a rich spectrum of (quasi-)liquid crystalline phases. The most interesting observation is the identification of stable smectic splay-bend ($S_{SB}$) and chiral smectic A ($S_A^*$) phases. The $S_{SB}$ phase is also stable in the limit, where only cis-conformers are allowed. The second phase occupying a considerable portion of the phase diagram is $S_A^*$ with chiral layers, where the chirality of the neighboring layers is of opposite sign. The study of the average fractions of the trans- and cis-conformers in various phases shows that while in the isotropic phase all fractions are equally populated, the $S_A^*$ phase is dominated by chiral conformers (zigzag), but the achiral conformers win in the smectic splay-bend phase. To clarify the possibility of stabilization of the nematic splay bend ($N_{SB}$) phase for trimers, the free energy of the $N_{SB}$ and $S_{SB}$ phases is calculated within DFT for the cis-conformers, for densities where simulations show stable $S_{SB}$. It turns out that the $N_{SB}$ phase is unstable away from the phase transition to the nematic phase, and its free energy is always higher than that of $S_{SB}$, down to the transition to the nematic phase, although the difference in free energies becomes extremely small when approaching the transition.

cond-mat.soft↗

arXiv2022

Splay-induced order in systems of hard wedges

We studied equilibrium systems composed of wedge-shaped monodisperse molecules using hard-particle Monte Carlo simulations. Each model molecule was made up of six colinear tangent spheres with linearly decreasing diameters. Thus, the shape was unequivocally described by a single parameter $d$: the ratio of the smallest and largest diameters of the spheres. The phases of the systems were analyzed as a function of $d$ and packing density $\eta$. As interactions were purely of the excluded volume type, the emergent phases were governed solely by the configurational entropy. For $\eta < 0.5$, in addition to the isotropic liquid, we observed standard nematic and smectic A liquid crystalline phases. However, for $\eta > 0.5$, apart from the ordinary non-polar hexagonal crystal, three new frustrated polar crystalline phases with splay modulation appeared: antiferroelectric splay crystal ($\text{Cr}_\text{S}\text{P}_\text{A}$), antiferroelectric double splay crystal ($\text{Cr}_\text{DS}\text{P}_\text{A}$) and ferroelectric double splay crystal ($\text{Cr}_\text{DS}\text{P}_\text{F}$). All configurations were studied in terms of nematic, smectic, and hexatic order parameters, as well as the radial distribution function and the polarization correlation function.

cond-mat.soft↗

arXiv2020

Twist-bend nematic phase from Landau-de Gennes perspective

The understanding of self-organization in the twist-bend nematic $(N_\text{TB})$ phase, identified in 2011 in liquid crystal dimers, is at the forefront of soft matter research worldwide. This new nematic phase develops structural chirality in the isotropic $(I)$ and the uniaxial nematic $(N_\text{U})$ phases, despite the fact that the molecules forming the structure are chemically achiral. Molecular, shape-induced flexopolarization provides a viable mechanism for a qualitative understanding of $N_\text{TB}$ and the related phase transitions. The key question that remains is whether with this mechanism one can also explain quantitatively the presently existing experimental data. To address this issue we propose a generalization of the mesoscopic Landau-de Gennes theory of nematics, where higher-order elastic terms of the alignment tensor are taken into account, in addition to the lowest-order flexopolarization coupling. The theory is not only capable of explaining the appearance of $N_\text{TB}$ but also stays in quantitative agreement with experimental data. In exemplary calculations, we take the data known for CB7CB flexible dimer - the "drosophila fly" in the studies of $N_\text{TB}$ [A. J\'{a}kli et al., Rev. Mod. Phys. 90, 045004 (2018)] - and estimate the constitutive parameters of the model from temperature variation of the nematic order parameter and the Frank elastic constants in the nematic phase. Then we seek for relative stability and properties of the isotropic, uniaxial nematic and twist-bend nematic phases. In particular, we evaluate various properties of $N_\text{TB}$, like temperature variation of the structure's wave vector, conical angle, flexopolarization, and remaining order parameters. We also look into the fine structure of $N_\text{TB}$, like its biaxiality - the property, which is difficult to access experimentally at the nanoscale.

cond-mat.soft↗

arXiv2017

Nematic twist--bend phase in an external field

Nematic twist--bend is the fifth nematic phase recognized in nature. This phase exhibits spiral orientational order, thus it is a chiral structure and it can be stabilized in systems composed of achiral molecules. The microscopic origin of this spontaneous chiral symmetry breaking is to a large extent unknown but phenomenologically it appears stabilized by assuming coupling between steric polar and orientational orderings. Understanding of how external fields affect the stability of this phase is of great intellectual interest and of relevance to potential applications. Within mesoscopic Landau--de Gennes theory we find that for compounds with positive anisotropy the helix unwinds to a polar uniaxial nematic, however negative material anisotropy gives rise to a rich sequence of new nematic phases obtained via mechanism of flattening the conical spiral.

cond-mat.soft↗

arXiv2016

Modulated nematic structures and chiral symmetry breaking in 2D

We have studied the properties of biaxial particles interacting via an anisotropic pair potential, involving second rank quadrupolar and third rank octupolar coupling terms, using Monte Carlo simulation. The particles occupy the sites of a 2D square lattice and the interactions are restricted to nearest neighbours. The system exhibits spontaneous chiral symmetry breaking from an isotropic phase to a chiral modulated nematic phase, composed of ambidextrous chiral domains. When two-fold axes of quadrupolar and octupolar tensors coincide this modulated phase appears to be the ambidextrous cholesteric phase of pitch comparable with a few lattice spacings, which can be regarded as a limiting case of the nematic twist bend phase. The associated phase transition is first-order.

cond-mat.soft↗

arXiv2016

Twist-bend nematic phases of bent-shaped biaxial molecules

How change in molecular structure can affect relative stability and structural properties of the twist-bend nematic phase (N$_\text{TB}$)? Here we extend the mean-field model [C. Greco et al., Soft Matter, 2014, 10, 9318] for bent-shaped achiral molecules, to study the influence of arm molecular biaxiality and the value of molecule's bend angle on relative stability of N$_\text{TB}$. In particular we show that by controlling biaxiality of molecule's arms up to four ordered phases can become stable. They involve locally uniaxial and biaxial variants of N$_\text{TB}$, together with the uniaxial and the biaxial nematic phases. However, the V-shaped molecule show stronger ability to form stable N$_\text{TB}$ than a biaxial nematic phase, where the latter phase appears in the phase diagram only for bend angles greater than $140^\circ$ and for large biaxiality of the two arms.

cond-mat.soft↗

arXiv2015

Modulated nematic structures induced by chirality and steric polarization

What kind of one-dimensional modulated nematic structures (ODMNS) can form nonchiral and chiral bent-core and dimeric materials? Here, using Landau-deGennes theory of nematics, extended to account for molecular steric polarization, we study a possibility of formation of ODMNS, both in nonchiral and intrinsically chiral liquid crystalline materials. Besides nematic and cholesteric phases, we find four bulk ODMNS for nonchiral materials, two of which have not been reported so far. These new structures are longitudinal ($N_{LP}$) and transverse ($N_{TP}$) periodic waves where the polarization field being periodic in one dimension stays parallel and perpendicular, respectively, to the wave vector. The other two phases have all characteristic features of the twist-bend nematic phase ($N_{TB}$) and the splay-bend nematic phase ($N_{SB}$), but their fine structure appears more complex than that considered so far. The presence of molecular chirality converts nonchiral $N_{TP}$ and $N_{SB}$ into new $N_{TB}$ phases. Interestingly, the nonchiral $N_{LP}$ phase can stay stable even in the presence of intrinsic molecular chirality. Exemplary phase diagrams provide further insights into the relative stability of these new modulated nematic structures.

cond-mat.soft↗

arXiv2015

Structure formation in monolayers composed of hard bent-core molecules

Two-dimensional ensembles of bent-core shaped molecules attain at highly orienting surfaces liquid crystalline structures characteristic mostly for lamellar chiral or nonchiral antiferroelectric order. Here, using the Onsager-type of density functional theory supplemented by constant-pressure Monte-Carlo (MC) simulation we investigate the role of excluded-volume interactions in stabilizing different structures in monolayers filled with bent-shaped molecules. We study influence of molecular features, like the apex angle, thickness of the arm and the type of the arm edges on the stability of layered structures. For simple molecular shapes taken the observed phases are dominated by the lamellar antiferroelectric type as observed experimentally, but a considerable sensitivity of the ordering to details of the molecular shape is found for order parameters and wave vectors of the structures. Interestingly, for large opening angles and not too thick molecules a window of stable nematic splay-bend phase is shown to exist. The presented theory models equilibrium properties of bent-core liquid crystals subjected to strong planar anchoring, in the case when details of the surface are of secondary importance.

cond-mat.soft↗

arXiv2010

Synchronization of Phase-coupled Oscillators with Distance-dependent Delay

By means of numerical integration we investigate the coherent and incoherent phases in a generalized Kuramoto model of phase-coupled oscillators with distance-dependent delay. Preserving the topology of a complete graph, we arrange the nodes on a square lattice while introducing finite interaction velocity, which gives rise to non-uniform delay. It is found that such delay facilitates incoherence and removes reentrant behavior found in models with uniform delay. A coupling-delay phase diagram is obtained and compared with previous results for uniform delay.

nlin.CD↗

arXiv2009

Stability of Biaxial Nematic Phase in Model Bent-Core Systems

We study a class of models for \sbentcore molecules using low density version of Local Density Functional Theory. Arms of the molecules are modeled using two- and three Gay-Berne (GB) interacting units of uniaxial and biaxial symmetry. Dipole-dipole interactions are taken into account by placing a dipole moment along the ${\mathcal{C}}_2$symmetry axis of the molecule. The main aim of the study is to identify molecular factors that can help stabilizing the biaxial nematic phase. The phase diagrams involving isotropic ($I$), uniaxial ($N_U$) and biaxial ($N_B$) nematic phases are determined at given density and dipole strength as function of bent angle. For molecules composed of two uniaxial arms a direct $I-N_B$ phase transition is found at a single Landau point, which moves towards lower bent angles with increasing dipole magnitude. For the three-segment model strengthening of the dipole-dipole interaction results in appearance of a line of Landau points. There exists an optimal dipole strength for which this line covers the maximal range of opening angles. Interestingly, the inclusion of biaxial GB ellipsoids as building blocks reveals the direct $I-N_B$ transitions line even in a non-polar, two-arms model. The line is shifted towards higher opening angles as compared to the uniaxial case.

cond-mat.soft↗

arXiv2009

Chiral Symmetry Breaking in Bent-Core Liquid Crystals

By molecular modeling we demonstrate that the nematic long-range order discovered in bent-core liquid crystal systems should reveal further spatially homogeneous phases. Two of them are identified as a tetrahedratic nematic ($N_T$) phase with $D_{2d}$ symmetry and a chiral tetrahedratic nematic ($N_T^*$) phase with $D_2$ symmetry. These new phases were found for a lattice model with quadrupolar and octupolar anisotropic interactions using Mean Field theory and Monte Carlo simulations. The phase diagrams exhibit tetrahedratic ($T$), $N_T$ and $N_T^*$ phases, in addition to ordinary isotropic ($I$), uniaxial nematic ($N_U$) and biaxial nematic ($N_B$) phases. To our knowledge, this is the first molecular model with spontaneous chiral symmetry breaking in non-layered systems.

cond-mat.soft↗

arXiv2007

Landau-deGennes Theory of Biaxial Nematics Re-examined

Recent experiments report that the long looked for thermotropic biaxial nematic phase has been finally detected in some thermotropic liquid crystalline systems. Inspired by these experimental observations we concentrate on some elementary theoretical issues concerned with the classical sixth-order Landau-deGennes free energy expansion in terms of the symmetric and traceless tensor order parameter $Q_{αβ}$. In particular, we fully explore the stability of the biaxial nematic phase giving analytical solutions for all distinct classes of the phase diagrams that theory allows. This includes diagrams with triple- and (tri-)critical points and with multiple (reentrant) biaxial- and uniaxial phase transitions. A brief comparison with predictions of existing molecular theories is also given.

cond-mat.soft↗

arXiv2007

Stability of Biaxial Nematic Phase for Systems with Variable Molecular Shape Anisotropy

We study the influence of fluctuations in molecular shape on the stability of the biaxial nematic phase by generalizing the mean field model of Mulder and Ruijgrok [Physica A {\bf 113}, 145 (1982)]. We limit ourselves to the case when the molecular shape anisotropy, represented by the alignment tensor, is a random variable of an annealed type. A prototype of such behavior can be found in lyotropic systems - a mixture of potassium laurate, 1-decanol, and $D_2O$, where distribution of the micellar shape adjusts to actual equilibrium conditions. Further examples of materials with the biaxial nematic phase, where molecular shape is subject to fluctuations, are thermotropic materials composed of flexible trimeric- or tetrapod-like molecular units. Our calculations show that the Gaussian equilibrium distribution of the variables describing molecular shape (dispersion force) anisotropy gives rise to new classes of the phase diagrams, absent in the original model. Depending on properties of the shape fluctuations, the stability of the biaxial nematic phase can be either enhanced or depressed, relative to the uniaxial nematic phases. In the former case the splitting of the Landau point into two triple points with a direct phase transition line from isotropic to biaxial phase is observed.

cond-mat.soft↗

arXiv2007

Synchronization in the presence of memory

We study the effect of memory on synchronization of identical chaotic systems driven by common external noises. Our examples show that while in general synchronization transition becomes more difficult to meet when memory range increases, for intermediate ranges the synchronization tendency of systems can be enhanced. Generally the synchronization transition is found to depend on the memory range and the ratio of noise strength to memory amplitude, which indicates on a possibility of optimizing synchronization by memory. We also point out on a close link between dynamics with memory and noise, and recently discovered synchronizing properties of networks with delayed interactions.

nlin.CD↗