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Nerea Sebastián

Publications and source records attributed to Nerea Sebastián.

At least 19 recordsLinked to original sources

Flexoelectricity-driven softening of bend elasticity leads to spontaneous chiral symmetry breaking in a polar fluid

The origin of the recently observed spontaneous chiral symmetry breaking in polar fluids composed of achiral molecules is an unsolved problem, raising fundamental questions about how heliconical structures emerge in such systems. Here, we investigate the pretransitional fluctuations leading to the formation of the spontaneously chiral twist-bend ferroelectric nematic phase using dielectric spectroscopy, light scattering, and small-angle X-ray scattering. We observe simultaneous softening of the bend elastic constant and the emergence of a collective dielectric mode on approaching the transition. By developing a theoretical model, we show that these phenomena are signatures of a flexoelectricity-driven transition arising from the coupling between electric polarization and bend deformation.

cond-mat.soft↗

Direct visualization of local electric fields in a layer of a ferroelectric nematic liquid

Ferroelectric nematic liquids exhibit complex ferroelectric domains shaped by competing elastic and electrostatic interactions. Using fluorescence and polarizing optical microscopy, we investigate domain formation and evolution under different anchoring conditions. Charged fluorescent ions map the electrostatic potential, revealing that electric fields are localized near domain walls and material surfaces. Upon cooling, domain walls transform from Ising- to Néel-type configurations, lowering the electrostatic potential, and reversibly recover upon heating.

cond-mat.soft↗

Elasticity-Driven Periodic Polarization Patterns in Confined Chiral Ferroelectric Nematic Fluid

Ferroelectric nematic phases are a new class of polar fluids in which spontaneous polarization is directly coupled to the orientational order, providing unique opportunities for creating self-organized materils with spatially modulated electric polarization and nonlinear optical response. Here we report the spontaneous emergence of polarization modulated textures in a chiral ferroelectric nematic material close to the transition to the chiral twist-bend ferroelectric nematic phase. By systematically varying cell thickness and surface anchoring conditions, we map the formation of these modulated states, revealing stripe, square and hexagonal morphologies determined via confinement conditions. These structures are directly translated into periodic modulation of the nonlinear optical response, as evidenced by second-harmonic generation imaging. Comparison with an elasticity based theoretical framework and numerical free energy minimization shows that the instability originates from the softening of the bend elastic constant in the chiral nematic phase as the system approaches the lower-temperature heliconical polar phase. The resulting elastic frustration, combined with confinement, drives the formation of spatially periodic director distortions, highlighting ferroelectric nematic fluids as a promising platform for self-assembled nonlinear optical materials.

cond-mat.soft↗

Modulated Anti-Ferroelectric Smectic Phases with Orthogonal and Tilted Structures

The discovery of the ferroelectric nematic phase has brought with it a plethora of new polar liquid crystalline phases. One in particular is the anti-ferroelectric smectic A SmA\textsubscript{AF} phase. In this letter we show via observation and analysis of satellite peaks in the X-ray scattering pattern that the structure of the SmA\textsubscript{AF} phase involves a density modulation of $\approx$10-20 nm lateral to the smectic layer normal. Further, we demonstrate a previously undiscovered phase where the anti-ferroelectric order is maintained into a tilted smectic phase demonstrating the robustness of the underlying frustration that leads to the modulated structure. We suggest that the modulations are only in a single dimension and appear parallel to the tilt plane. This new phase also shows a significantly different and complex response to an electric field from other discovered polar LC phases due to the ability to modulate both tilt and polarisation direction.

cond-mat.soft↗

Nanostructured multiferroic liquids: on the way to fluid ferroelectric magnets

Responsiveness to multiple stimuli and adaptivity are paramount for designing smart multifunctional materials. In soft, partially ordered systems, these features can often be achieved via self-assembly, allowing for the combination of diverse components in a complex nanostructured material. Here, we demonstrate an example of a liquid that simultaneously displays both ferroelectric and ferromagnetic types of order. This material is a nanostructured liquid crystalline hybrid comprising ferrimagnetic barium hexaferrite nanoplatelets suspended in a ferroelectric nematic host. Director-mediated interactions drive the self-assembly of nanoplatelets in an intricate network. Due to the couplings between the polar electric and magnetic types of order, this material demonstrates magnetically driven electric and nonlinear optical responses, as well as electrically driven magnetic response. Such multiferroic liquids are highly promising for applications in energy harvesting, nonlinear optics, and sensors.

cond-mat.soft↗

Antiferroelectric order in nematic liquids: Flexoelectricity vs electrostatics

The recent discovery of ferroelectric nematic liquid crystalline phases marks a major breakthrough in soft matter research. An intermediate phase, often observed between the nonpolar and the ferroelectric nematic phase, shows a distinct antiferroelectric response to electric fields. However, its structure and formation mechanisms remain debated, with flexoelectric and electrostatics effects proposed as competing mechanisms. By controlling the magnitude of electrostatic forces through ion addition in two representative ferroelectric nematic materials, we show that the primary mechanism for the emergence of antiferroelectric order is the flexoelectric coupling between electric polarization and splay deformation of the nematic director. The addition of ions significantly expands the temperature range over which the antiferroelectric phase is observed, with this range increasing with increasing ion concentration. Polarizing optical microscopy studies and second harmonic generation microscopy reveal the splayed structure modulated in two dimensions, while SHG interferometry confirms its antiferroelectric character. We extend the model previously used to describe pretransitional behaviour by incorporating the electrostatic contribution of ions. The model shows qualitative agreement with the experiments, accurately reproducing the phase diagram and temperature-dependent evolution of the modulation period of the observed structure.

cond-mat.soft↗

Tuneable entangled photon pair generation in a liquid crystal

Liquid crystals, with their ability of self-assembly, strong response to the electric field, and integrability into complex systems, are key materials in light beam manipulation. Recently discovered ferroelectric nematic liquid crystals also possess a considerable second-order optical nonlinearity, making them a perspective material for nonlinear optics. Their use as sources of quantum light could drastically extend the boundaries of photonic quantum technologies. However, spontaneous parametric down-conversion, the basic source of entangled photons, heralded single photons, and squeezed light, has been so far not observed in liquid crystals - or in any liquids or organic materials. Here, we implement spontaneous parametric down-conversion in a ferroelectric nematic liquid crystal and demonstrate electric-field tunable broadband generation of entangled photons, with the efficiency comparable to that of the best nonlinear crystals. The emission rate and polarization state of photon pairs is dramatically varied by applying a few volts or twisting the molecular orientation along the sample. A liquid crystal source enables a new type of quasi-phasematching, which is based on molecular twist structure and is therefore reconfigurable for the desired spectral and polarization properties of photon pairs. Such sources promise to outperform standard nonlinear optical materials in terms of functionality, brightness and the tunability of the generated quantum state. The concepts developed here can be extended to complex topological structures, macroscopic devices, and multi-pixel tunable quantum light sources.

physics.optics↗

A molecular perspective on the emergence of long-range polar order from an isotropic fluid

The ferroelectric nematic phase (N$_{\text{F}}$) has quickly become the most studied system in liquid crystal research. In this work, we investigate the origin of such polar structure by studying a compound for which the N$_{\text{F}}$ phase directly follows the isotropic liquid phase on cooling, making it a particularly interesting system. Our experimental results evidence the presence of polar correlations already in the high-temperature phase, in which ferroelectric order can be induced under a sufficiently strong electric field. In the N$_{\text{F}}$ phase, molecular dynamics and polar correlations are investigated through detailed dynamic dielectric measurements, while second harmonic generation experiments evidence a large value of the main coefficient of the second order dielectric susceptibility tensor. Lastly, experimentally determined parameters are employed for calculations based on a recently proposed theoretical model for the stability of the N$_{\text{F}}$ phase. The obtained results suggest that the parallel alignment of dipoles is driven by a subtle interplay between electrostatic and excluded volume interactions.

cond-mat.soft↗

Isotropic to nematic transition in alcohol ferrofluids of barium hexaferrite nanoplatelets

Alcohol ferrofluids made of ferrimagnetic barium hexaferrite (BHF) nanoplatelets (NPLs) form a unique example of a dipolar fluid - a liquid magnet. Its formation is induced at a high enough concentration of the NPLs. The key interactions between the NPLs are long-ranged dipolar magnetic and screened anisotropic electrostatic. Herein, we report the results on tuning the isotropic-nematic phase transition (i.e., the NPLs threshold concentration) in 1-butanol ferrofluids of BHF NPLs by affecting the interactions in the ferrofluids. The threshold concentration was determined by polarizing optical microscopy (POM) combined with a system for magnetic field manipulation and was in the range between 4.6 and 6.6 \% (v/v) depending on the ferrofluid. We observed that the threshold concentration decreased for 0.6 \% (v/v) with a larger mean diameter of the NPLs, up to 0.6 \% (v/v) with increased ionic strength of the ferrofluid, and for $\sim$ 2 \% (v/v) with higher saturation magnetization of the NPLs. We showed that by tuning the parameters affecting the ferrofluid's interplatelet interactions, we can alter the threshold concentration for the liquid magnet formation. The results elucidate the importance of a delicate balance between the repulsive screened electrostatic and attractive dipolar magnetic interactions for the liquid magnet formation.

cond-mat.soft↗

Dielectric spectroscopy of a ferroelectric nematic liquid crystal and the effect of the sample thickness

The recently discovered ferroelectric nematic liquid crystals have been reported to exhibit very large dielectric permittivity values. Here, we report a systematic investigation of the dielectric behavior of a prototypical ferroelectric nematogen by varying the thickness of the parallel capacitor measuring cell. While in the non-polar high temperature nematic phase results show only slight differences due to slight variations of the alignment, the measured permittivity values in the ferroelectric nematic phase show a linear dependence on the cell thickness. It is also shown that the characteristic relaxation frequency decreases inversely proportionally to the thickness. The results are discussed in terms of three different available models based on different underlying mechanisms, accounting for cancellation of the probe electric fields by polarization reorientation or by ionic charges, or based on a recently proposed continuous phenomenological model.

cond-mat.soft↗

Collective and non-collective molecular dynamics in a ferroelectric nematic liquid crystal studied by broadband dielectric spectroscopy

A great deal of effort has been recently devoted to the study of dielectric relaxation processes in ferroelectric nematic liquid crystals, yet their interpretation remains unclear. In this work, we present the results of broadband dielectric spectroscopy experiments of a prototypical ferroelectric nematogen in the frequency range 10 Hz-110 MHz at different electrode separations and under the application of DC bias fields. The results evidence a complex behavior in all phases due to the magnitude of polar correlations in these systems. The observed modes have been assigned to different relaxation mechanisms based on existing theoretical frameworks.

cond-mat.soft↗

Polarization patterning in ferroelectric nematic liquids

The recently discovered ferroelectric nematic liquids incorporate to the functional combination of fluidity, processability and anisotropic optical properties of nematic liquids, an astonishing range of physical properties derived from the phase polarity. Among them, the remarkably large values of second order optical susceptibility encourage to exploit these new materials for non-linear photonic applications. Here we show that photopatterning of the alignment layer can be used to structure polarization patterns. To do so, we take advantage of the flexoelectric effect and design splay structures that geometrically define the polarization direction. We demonstrate the creation of periodic polarization structures and the possibility of guiding polarization by embedding splay structures in uniform backgrounds. The demonstrated capabilities of polarization patterning, open a promising new route for the design of ferroelectric nematic based photonic structures and their exploitation.

cond-mat.soft↗

Role of ionic surfactant in magnetic dynamics of self-assembled dispersions of nanoplatelets

In complex colloidal systems, interparticle interactions strongly affect the dynamics of the constituting particles. A study of the dynamical response also provides invaluable information on the character of those interactions. Here we demonstrate how tuning the electrostatic interactions by an ionic surfactant in dispersions of magnetic nanoplatelets leads to developing new dynamic modes in magnetic response spectra. The collective modes can be induced or suppressed by either varying the concentration ratio of the magnetic nanoplatelets (MP) to the surfactant or increasing the MP concentration reflecting the nanoscale characteristics of this fluid magnet.

cond-mat.soft↗

Running streams of a ferroelectric nematic liquid crystal on a lithium niobate surface

Sessile droplets of a ferroelectric nematic liquid crystalline material were exposed to surface electric fields produced by pyroelectric and photogalvanic (photovoltaic) effects in X-cut iron-doped lithium niobate crystals. The resulting dynamic processes were monitored by polarization optical (video)microscopy (POM). During heating/cooling cycles, at first, the droplets change their shape from spherical to extended ellipsoidal. Then they start to move rapidly along the surface electric field, i.e., along the crystal's polar axis (c-axis). During this motion, several droplets merge into running streams (tendrils) extending towards the edges of the top surface area. Finally, practically all liquid crystalline material is transported from the top surface to the side surfaces of the crystal. At stabilized temperature, laser illumination of the assembly causes dynamic processes that are localized to the illuminated area. Also, in this case, the LC droplets merge into several tendril-like formations that are preferentially oriented along the c-axis of the crystal. The pattern of tendrils fluctuates with time, but it persists as long as the illumination is present. In this case, the LC material is transported between the central and the edge region of the illuminated area.

cond-mat.soft↗

Light-induced dynamics of liquid-crystalline droplets on the surface of iron-doped lithium niobate crystals

We investigated the effect of a photovoltaic field generated on the surface of iron-doped lithium niobate crystals on droplets of a ferroelectric nematic liquid crystalline and a standard nematic liquid crystalline material deposited on this surface. When such assembly is illuminated with a laser beam, a wide range of dynamic phenomena are initiated. Droplets located outside the laser spot are dragged in the direction of the illuminated area, while droplets located inside the illuminated region tend to bridge each other and rearrange into tendril-like structures. In the ferroelectric nematic phase (NF) these processes take place via the formation of conical spikes evolving into jet streams, similar to the behavior of droplets of conventional dielectric liquids exposed to overcritical electric fields. However, in contrast to conventional liquids, the jet streams of the NF phase exhibit profound branching. In the nematic phase (N) of both the ferroelectric nematic and the standard nematic material, dynamic processes occur via smooth-edged continuous features typical for conventional liquids subjected to under-critical fields. The difference in dynamic behavior is attributed to the large increase of dielectric permittivity in the ferroelectric nematic phase with respect to the dielectric permittivity of the nematic phase.

cond-mat.soft↗

Ferroelectric nematic liquid crystalline phases

Recent experimental realization of ferroelectric nematic liquid crystalline phases stimulated material development and numerous experimental studies of these new phases, guided by their fundamental and applicative interest. In this Perspective, we give an overview of this emerging field by linking history and theoretical predictions to a general outlook of the development and properties of the materials exhibiting ferroelectric nematic phases. We will highlight the most relevant observations up-to-date, e.g., giant dielectric permittivity values, polarization values an order of magnitude larger than in classical ferroelectric liquid crystals, and nonlinear optical coefficients comparable to several ferroelectric solid materials. Key observations of anchoring and electro-optic behavior will also be examined. The collected contributions lead to a final discussion on open challenges in materials development, theoretical description, experimental explorations, and possible applications of the ferroelectric phases.

cond-mat.soft↗

Electrooptics of mm-scale polar domains in the ferroelectric splay nematic phase

The recent discovery of the ferroelectric splay nematic phase has opened the door to experimental investigation of one of the most searched liquid crystal phases in decades, with high expectations for future applications. However, at this moment, there are more questions than answers. In this work, we examine the formation and structure of large polar nematic domains of the ferroelectric splay nematic material RM734 in planar liquid crystals cells with different aligning agents and specifications. We observe that confining surfaces have a strong influence over the formation of different types of domains, resulting in various twisted structures of the nematic director. For those cells predominantly showing mm-scale domains, we investigate the optical and second harmonic generation switching behaviour under applications of electric fields with a special focus on in-plane fields perpendicular to the confinement media rubbing direction. In order to characterize the underlying structure, the polar optical switching behaviour is reproduced using a simplified model together with Berreman calculations.

cond-mat.soft↗

On the molecular origins of the ferroelectric splay nematic phase

Nematic liquid crystals have been known for more than a century, but it was not until the 60s-70s that, with the development of room temperature nematics, they became widely used in applications. Polar nematic phases have been long-time predicted, but have only been experimentally realized recently. Synthesis of materials with nematic polar ordering at room temperature is certainly challenging and requires a deep understanding of its formation mechanisms, presently lacking. Here, we compare two materials of similar chemical structure and demonstrate that just a subtle change in the molecular structure enables denser packing of the molecules when they exhibit polar order, which shows that reduction of excluded volume is in the origin of the polar nematic phase. Additionally, we propose that molecular dynamics simulations are potent tools for molecular design in order to predict, identify and design materials showing the polar nematic phase and its precursor nematic phases.

cond-mat.soft↗