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Physics Condensed Matter Soft Condensed Matter

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Monday 3 August

Soft Condensed Matter

Equilibrium gigahertz acoustics reveals long-range confinement in liquids

Understanding how the mechanical properties of liquids confined within nanometer-scale gaps differ from bulk behavior is central to biophysics, lubrication, catalysis, electrochemistry, and surface science. Yet the characterization of ultrathin confined liquids remains challenging, as many existing approaches rely on destructive or intrusive contact-based techniques, mostly measuring the liquid flow in the low frequency regime. Here, we present a non-invasive, all-optical technique based on ultrafast laser ultrasonics that probes confined liquids at equilibrium in the gigahertz frequency range. The method measures the phase and amplitude of time-domain Brillouin scattering signals transmitted through liquid layers whose thickness is varied step by step with subnanometer effective sampling. Supported by numerical modeling of acoustic propagation and optical detection, these signals allow us to extract the thickness-dependent acoustic velocity and attenuation of confined liquids. We show that nanometric confinement modifies the GHz acoustic response of glycerol, the liquid crystal 8CB, and a butyl-based ionic liquid over unexpectedly long spatial scales. These effects extend from a few nanometers to several tens of nanometers and reveal bound interfacial layers, acoustic stiffening, and enhanced solid-like behavior under confinement. Our results open a route to probing liquid confinement in a scarcely explored regime: dynamically measured at gigahertz frequencies, yet sufficiently weakly perturbative to preserve the equilibrium confined state.
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Soft Condensed Matter

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.
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All authors Anej Sterle, Natan Osterman, Calum J. Gibb, Jordan Hobbs, Richard J. Mandle, Nerea Sebastián, Alenka Mertelj

Soft Condensed Matter · Cross-listed from cond-mat.mes-hall

Complete Structural Determination of Mesostructural Dodecagonal Quasicrystalline Particles

Quasicrystals have revolutionized our understanding of order in solids by demonstrating exotic structural and physicochemical properties with diverse potential applications. Despite the development of various theoretical models and experimental techniques to describe quasicrystal structures, the precise determination of local three dimensional (3D) arrangements of constituent atoms, or of secondary building units such as clusters or micelles, remains elusive. This challenge is particularly acute in self assembled soft matter quasicrystalline systems, where the complex assembly of molecular groups introduces additional defects and structural modulations. Herein, we report the first complete structural determination of self-assembled mesostructural dodecagonal quasicrystalline particles. Employing advanced electron tomography, combined with dedicated structural tracing and processing workflows, the 3D coordinates of all nodal sites were extracted. This approach reveals that the actual structure deviates from the conventionally assumed tetrahedral close packing geometry, exhibiting diverse coordination environments and displacive fluctuations. We identified and quantified rotational intergrowths arising from node exchange, as well as various defects and disorder, with these features discernible only through 3D analysis. Additionally, we propose a simplified two-layer stacking of isomorphic hexagonal model to form dodecagonal quasicrystal. This work advances our understanding of soft-matter dodecagonal quasicrystals and paves the way for detailed structural elucidation of self-assembled systems.
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All authors Xueliang Zhang, Xi Wang, Nobuhisa Fujita, Osamu Terasaki, Lu Han

Soft Condensed Matter

A numerical study to analyze the interplay of Weissenberg number and viscosity ratio in a log-strain tensorial model for viscoelastic fluids

We present a computational study aimed at exploring the different and independent roles of the Weissenberg number and of the ratio between the polymeric and solvent viscosity contributions in a viscoelastic fluid model. The tensorial model under investigation, recently proposed, is based on a logarithmic relation between the elastic (or recoverable) strain and the elastic stress. In this model, the elastic strain plays the role of a conformation tensor and its evolution equation inherently preserves its determinant and positive definiteness. These properties are also enforced in the computational method employed in the study. A finite-difference discretization in time is combined with a stabilized mixed finite element formulation based on the Variational Multiscale method for the spatial discretization and with a generalized Lie derivative approach for the advection terms. The behavior of the model is analyzed in paradigmatic pressure-driven flows and we find that the value of the viscosity ratio is crucial in determining to which extent non-Newtonian flow profiles are observed upon increasing the Weissenberg number. By comparing the solutions of the log-strain tensorial model with those of a suitable Generalized Newtonian Fluid model, we show that flow-type dependence plays a significant role even in the simple planar flow past a cylinder.
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Soft Condensed Matter

Fluid-structure coupling governs a dynamic transition in foam scraping

Foam scraping exhibits a dynamic transition between a slip state, in which the foam moves beneath a plate, and a scraping state, in which the foam is expelled from the confined region. Although this transition has been associated with the propagation of local T1 rearrangements, the physical parameter controlling their propagation remains unclear. Here, we investigate the dependence of the critical scraping velocity on the liquid fraction, bulk viscosity, and surfactant system. For all examined conditions, the critical capillary number follows $\mathrm{Ca}_c\propto\phi^{-1}$, apart from a solution-dependent prefactor. We propose a local fluid–structure-coupling model in which viscous work transmitted through the Plateau-border network competes with the effective energetic cost required for one T1 event to trigger the next. The observed scaling implies an effective energetic cost governed by the Laplace pressure and is consistent with a small local compressive component of the bubble deformation. These results identify local coupling between interstitial flow and bubble deformation as a mechanism controlling the macroscopic slip–scraping transition.
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Soft Condensed Matter

Impedance of an electric double layer capacitor with a multi-component electrolyte

I derive the impedance response of an ideal electrolyte containing an arbitrary number of mobile ionic species between blocking planar electrodes, described by the Poisson–Nernst–Planck equations. By transforming the linearized equations to a charge–salt basis, the response is written in terms of a multi-component diffusion–migration matrix and its eigenvalues/eigenvectors. When all diffusivities are equal, the charge mode decouples from the neutral concentration subspace and the classical binary-electrolyte result is recovered. In contrast, unequal diffusivities couple charge relaxation to one or more neutral composition modes. For a ternary electrolyte with two cations and one anion, this coupling produces additional diffusive features and broadens the crossover between resistive and capacitive regimes. The results found in this paper provide a minimal continuum explanation for why mixed electrolytes can display impedance spectra that cannot be interpreted as a simple binary electrolyte with an averaged diffusion coefficient.
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