arXiv subjects

Kyohei Takae

Publications and source records attributed to Kyohei Takae.

At least 19 recordsLinked to original sources

arXiv2026

Liquid-state structural asymmetry governs species-selective crystallization in multicomponent systems

Multicomponent crystals are often assumed to form nearly random solid solutions when thermodynamically stable. However, crystal growth proceeds from structurally heterogeneous liquids, raising the possibility that the liquid state may influence which species are incorporated into the growing crystal. Here we demonstrate that liquid-state structural asymmetry can induce species-selective crystallization in multicomponent systems. Using molecular dynamics simulations of a multivalent rocksalt-type model (AgPbBiTe$_3$), we find that cations with higher valence readily form locally crystal-compatible coordination environments in the liquid and are efficiently incorporated into the growing lattice, whereas lower-valence cations exhibit more disordered liquid coordination and attach less efficiently at the crystal-liquid interface. This asymmetry leads to species-selective incorporation and slower crystal growth. Depth-resolved photoelectron spectroscopy measurements on AgPbBiTe$_3$ further reveal enhanced Ag concentration near grain-boundary and surface regions, consistent with the selective incorporation predicted by the simulations. These results demonstrate that structural compatibility between liquid-state structure and the target crystal motif governs selective incorporation during crystallization, providing a general kinetic mechanism by which compositional heterogeneity can emerge during growth of multicomponent crystals.

cond-mat.soft↗

arXiv2025

Elastic heterogeneity governs anomalous scaling in a soft porous crystal

Nanoscale molecular transport plays a crucial role in regulating mass diffusion and responsiveness in condensed matter systems. In soft porous crystals, in particular, adsorption of guest molecules induces host framework deformation and changes in rigidity, underpinning their characteristic stimuli-responsive behaviour. Surface-mediated adsorption leads to inhomogeneous adsorbate distribution, which, through local framework deformation, induces spatial variations in rigidity -- elastic heterogeneity. Although this heterogeneity is expected to affect adsorption kinetics and mechanical behaviour, its role remains poorly understood. Here we show that elastic heterogeneity governs adsorption kinetics, leading to emergent phenomena including size-dependent uptake, surface creasing, and anomalous dynamic scaling that is distinct from established scaling. Stress relaxation near corners facilitates adsorption, resulting in a size-dependent deviation from diffusive kinetics. Away from corners, flexible unadsorbed regions between rigid adsorbed domains relieve stress through crease formation. The resulting lateral correlations exhibit anomalous dynamic scaling, characterized by a breakdown of scale invariance between global and local interfacial fluctuations. These findings provide a mechanistic foundation for controlling adsorption and deformation kinetics in soft porous materials via elastic heterogeneity. Our work opens a route to engineering responsive materials, where mechanical feedback is harnessed to control cooperative molecular transport and drive macroscopic shape changes under external perturbations.

cond-mat.soft↗

arXiv2025

Cooperative Ion Conduction Enabled by Site Percolation in Random Substitutional Crystals

Efficient and safe energy storage technologies are essential for realizing a sustainable and electrified society. Among the key challenges, the design of superionic conductors for all-solid-state batteries often faces a fundamental trade-off between stability and ionic conductivity. Random substitutional crystals, where atomic species are randomly distributed throughout a crystal lattice, present a promising route to overcome this trade-off. Although the importance of cooperative motion in ion conduction has been pointed out, there is a lack of understanding of the relationship between mesoscale structural organization and macroscopic conductivity, limiting the rational design of optimal compositions. Here, we systematically investigate the ionic conductivity of rock salt random substitutional ionic crystals Li$_x$Pb$_{1-2x}$Bi$_x$Te as a function of Li concentration $x$ using molecular dynamics simulations. We find that ionic conductivity increases sharply once the $x$ exceeds a critical threshold, without disrupting the underlying crystal structure. Strikingly, this threshold aligns with the site-percolation threshold predicted by percolation theory. Our findings establish ion percolation as a universal design principle that reconciles the trade-off between conductivity and stability, offering a simple and broadly applicable strategy for the development of robust, high-performance solid electrolytes.

cond-mat.mtrl-sci↗

arXiv2024

Spontaneous formation of Frenkel defects in high-entropy-alloys-type compound

High-entropy alloys (HEAs) are attracting attention due to their exceptional properties, such as enhanced mechanical toughness, superconducting robustness, and thermoelectric performance. Numerous HEAs have been developed for diverse applications, ranging from self-healing in fusion reactors to addressing environmental concerns with thermoelectric materials. Understanding atomic diffusion within HEA crystals is crucial for these applications. Here, this study investigates diffusion mechanisms in PbTe-based HEAs, focusing on the role of indium (In). Molecular dynamics simulations reveal that In inclusion prompts spontaneous Frenkel defect formation, notably enhancing diffusion not only of In$^+$ but also other cations. Frenkel defect formation, closely linked to alloy properties, is predominantly influenced by charge rather than cation size. This insight not only enhances comprehension of HEA diffusion mechanisms but also develops HEAs with properties such as self-healing from damage and high ion permeability, advancing the field of material science.

cond-mat.mtrl-sci↗

arXiv2023

Adsorption superlattice stabilized by elastic interactions in a soft porous crystal

We numerically show that molecules adsorbed in a soft porous crystal form a superlattice (SL) stabilized by elastic interactions. In a mechanically flexible honeycomb lattice model, when the elastic interactions between the next nearest neighboring lattice sites are strong, a long-range ordered 1/3-filling SL state emerges. By calculating the thermodynamic stability, it is found that the SL state is robust against thermal fluctuation. Our results provide a mechanism of elasticity-driven SL formation, which can be utilized for controlling the distribution of adsorbed molecules.

cond-mat.soft↗

arXiv2023

Elastic heterogeneity governs asymmetric adsorption-desorption in a soft porous crystal

Metal--organic frameworks (MOFs), which possess a high degree of crystallinity and a large surface area with tunable inorganic nodes and organic linkers, exhibit high stimuli-responsiveness and molecular adsorption selectivity that enable various applications. The adsorption in MOFs changes the crystalline structure and elastic moduli. Thus, the coexistence of adsorbed/desorbed sites makes the host matrices elastically heterogeneous. However, the role of elastic heterogeneity in the adsorption--desorption transition has been overlooked. Here we show the asymmetric role of elastic heterogeneity in the adsorption--desorption transition. We construct a minimal model incorporating adsorption-induced lattice expansion/contraction and an increase/decrease in the elastic moduli. We discover that the transition is hindered by the entropic and energetic effects which become asymmetric in adsorption process and desorption process, leading to the strong hysteretic nature of the transition. Furthermore, the adsorbed/desorbed sites exhibit spatially heterogeneous domain formation, implying that the domain morphology and interfacial area between adsorbed/desorbed sites can be controlled by elastic heterogeneity. Our results provide a theoretical guideline for designing soft porous crystals with tunable adsorption hysteresis and the dispersion and domain morphology of adsorbates using elastic heterogeneity.

cond-mat.soft↗

arXiv2023

Diffusionless relaxation of half-skyrmion liquid, hexatic, and crystalline states in a chiral molecular crystal

Particles in a crowded environment exhibit slow anomalous diffusion, and their efficient manipulation is important in controlling transport phenomena in complex materials. Skyrmions and half-skyrmions, spatially localized quasiparticles observed in magnetic systems and liquid crystals, also exhibit diffusive motion. They exhibit normal diffusion in dilute conditions. However, the cooperative dynamics and diffusion of skyrmions and half-skyrmions in their condensed liquid, hexatic, and crystalline phases are elusive. Here we show in the half-skyrmion condensed phases that the fusion and fission of half-skyrmions, not their diffusion, are responsible for the primary structural relaxation. The fusion and fission occur due to the non-conserved nature of the quasiparticle number density. The diffusion, which contributes to the secondary structural relaxation, is suppressed by cages formed by surrounding half-skyrmions, whereas enhanced by Mermin-Wagner fluctuation characteristic to two-dimensional systems, leading to subdiffusive motion. Large displacement of half-skyrmions is locally excited by fusion-fission and bond-breaking between adjacent half-skyrmions via heterogeneous elastic fields. Furthermore, the motion of half-skyrmions couples with transverse and longitudinal sound wave excitation differently, where the transverse sound wave is more attenuated than the longitudinal one due to the coupling between transverse sound wave and half-skyrmion deformation. We also discuss the {relationship} between half-skyrmion diffusion in our system and skyrmion diffusion in magnetic systems. Our result provides a qualitative difference in dynamical properties between half-skyrmion gaseous and condensed phases, suggesting the efficient manipulation of high-density half-skyrmions and skyrmions.

cond-mat.soft↗

arXiv2022

Glassy atomic vibrations and blurry electronic structures created by local structural disorders in high-entropy metal telluride superconductors

The motivation of this work is our recent observation of the robustness of superconductivity in a High-entropy (HE) superconductor Ag0.2In0.2Sn0.2Pb0.2Bi0.2Te (CsCl-type) to external pressure. The superconducting transition temperature (Tc) of Ag0.2In0.2Sn0.2Pb0.2Bi0.2Te is almost constant with pressure, described as robustness of superconductivity to pressure, whereas the PbTe with zero configurational entropy of mixing exhibits a clear decrease in Tc with pressure. Here, we investigated the atomic displacement parameters (Uiso), the atomic-vibration characteristics, and the electronic states of metal tellurides (MTe) with various configurational entropy of mixing (DSmix) at the M site. The Uiso for the M site is clearly increased by M-site alloying with DSmix > 1.1R, which is the evidence of local disorder introduced by the increase in DSmix via the solution of three or more M elements. The revealed vibrational density of states (DOS) shows a remarkable broadening with DSmix > 1.1R, which indicates glassy characteristics of atomic vibration in HE MTe with a NaCl-type structure (low-pressure phase). On the electronic states of the CsCl-type (high-pressure) phases, where the robustness of Tc is observed, blurry electronic band structure appears with increasing DSmix, which indicates the evolution of blurry (glassy) electronic states in HE MTe with the CsCl-type structure. The estimated electronic DOS at Fermi energy cannot explain the changes in Tc for HE MTe when assuming conventional electron-phonon superconductivity, but the conventional explanation seems to work for PbTe. Therefore, the pairing mechanisms in MTe with DSmix > 1.1R are affected by glassy phonon and/or blurry electronic states in MTe, and the robustness of superconductivity would be originating from unique electron-phonon coupling.

cond-mat.supr-con↗

arXiv2021

Emergent elasticity linked to topological phase transitions controlled via molecular chirality and steric anisotropy

Self-organisation into spatially modulated structures has different nature from phase transition into uniform states. Skyrmions and half-skyrmions (merons) are representatives of such structures and are utilised in designing magnetoelectric, optical, and mechanoresponsive materials by controlling topological phases. However, skyrmions and half-skyrmions in molecular solids are rarely studied, though there is a universality in theoretical descriptions between magnetic and molecular systems with chiral interactions. Here we develop a simple physical system for controlling topological phases in a solid with chirality. We reveal that emergence of elastic fields from anisotropic steric interactions and intermolecular twisting is a key to control helical and half-skyrmion structures. Utilising the coupling between the emergent elastic fields and molecular orientations, we successfully control topological phases by temperature, external electromagnetic fields, and anisotropic stresses. The concept of the emergent elasticity provides a control system for designing molecular and macromolecular solids with tunable electro- and magneto-mechanical properties.

cond-mat.mtrl-sci↗

arXiv2020

Phase separation kinetics of a symmetric binary mixture of glass-forming liquids

Mixtures of glass-forming fluids sometimes exhibit glass-glass phase separation at low temperatures. Here, we use a molecular dynamics simulation to study one of the simplest examples of the glass-glass phase separation. We consider a mixture composed of type A and B particles, in which the A-A and B-B interactions are the identical Lennard-Jones interactions and the A-B interaction is repulsive only. To avoid crystallization, we also introduce the polydispersity in the particle sizes for each component. We study the phase separation kinetics of this model at a 50:50 concentration at various temperatures. We find that hydrodynamic coarsening takes place when the temperature is higher than the onset temperature of the glassy dynamics. At lower temperatures, diffusive coarsening is observed over a long duration, and a further slower coarsening appears within a shorter time. Below the glass transition temperature, the domain growth does not stop but becomes logarithmically slow or even slower than logarithmic. By analyzing two-time correlation functions, we show that these slow coarsening processes are accompanied by a slowing down of the microscopic dynamics, which has qualitative similarities with the aging dynamics without phase separation. Based on the results, we discuss a possible link between the slow coarsening and the aging-like microscopic slowing down in the glass-glass phase separation.

cond-mat.stat-mech↗

arXiv2017

Ferroelectric glass of spheroidal dipoles with impurities: Polar nanoregions, response to applied electric field, and ergodicity breakdown

Using molecular dynamics simulation, we study dipolar glass in crystals composed of slightly spheroidal, polar particles and spherical, apolar impurities between metal walls. We present physical pictures of ferroelectric glass, which have been observed in relaxors, mixed crystals (such as KCN$_x$KBr$_{1-x}$), and polymers. Our systems undergo a diffuse transition in a wide temperature range, where we visualize polar nanoregions (PNRs) surrounded by impurities. In our simulation, the impurities form clusters and their space distribution is heterogeneous. The polarization fluctuations are enhanced at relatively high $T$ depending on the size of the dipole moment. They then form frozen PNRs as $T$ is further lowered into the nonergodic regime. As a result, the dielectric permittivity exhibits the characteristic features of relaxor ferroelectrics. We also examine nonlinear response to cyclic applied electric field and nonergodic response to cyclic temperature changes (ZFC$/$FC), where the polarization and the strain change collectively and heterogeneously. We also study antiferroelectric glass arising from molecular shape asymmetry. We use an Ewald scheme of calculating the dipolar interaction in applied electric field.

cond-mat.soft↗

arXiv2015

Fluctuations of local electric field and dipole moments in water between metal walls

We examine the thermal fluctuations of the local electric field $E_k^{\rm loc}$ and the dipole moment $μ_k$ in liquid water at $T=298$ K between metal walls in electric field applied in the perpendicular direction. We use analytic theory and molecular dynamics simulation. In this situation, there is a global electrostatic coupling between the surface charges on the walls and the polarization in the bulk. Then, the correlation function of the polarization density $p_z(r)$ along the applied field contains a homogeneous part inversely proportional to the cell volume $V$. Accounting for the long-range dipolar interaction, we derive the Kirkwood-Fr$\ddot{\rm{o}}$hlich formula for the polarization fluctuations when the specimen volume $v$ is much smaller than $V$. However, for not small $v/V$, the homogeneous part comes into play in dielectric relations. We also calculate the distribution of $E_k^{\rm loc}$ in applied field. As a unique feature of water, its magnitude $|E_k^{\rm loc}|$ obeys a Gaussian distribution with a large mean value $E_0 \cong 17~$V$/$nm, which arises mainly from the surrounding hydrogen-bonded molecules. Since $|μ_k|E_0\sim 30 k_{\rm B}T$, $μ_k$ becomes mostly parallel to $E_k^{\rm loc}$. As a result, the orientation distributions of these two vectors nearly coincide, assuming the classical exponential form. In dynamics, the component of $μ_k(t)$ parallel to $E_k^{\rm loc}(t)$ changes on the timescale of the hydrogen bonds $\sim 5$ ps, while its smaller perpendicular component undergoes librational motions on timescales of 0.01 ps.

cond-mat.soft↗

arXiv2015

Molecular Dynamics Simulation of Water between Metal Walls under Electric Field: Dielectric Response and Dynamics after Field Reversal

We study water between parallel metal walls under applied electric field accounting for the image effect at $T=298$ K. The electric field due to the surface charges serves to attract and orient nearby water molecules, while it tends to a constant determined by the mean surface charge density away from the walls. We find Stern boundary layers with thickness about $5$ $\rm Å$ and a homogeneously polarized bulk region. The molecules in the layers more sensitively respond to the applied field than in the bulk. As a result, the potential drop in the layers is larger than that in the bulk unless the cell length exceeds 10 nm. We also examine the hydrogen bonds, which tend to make small angles with respect to the walls in the layers even without applied field. The average local field considerably deviates from the classical Lorentz field and the local field fluctuations are very large in the bulk. If we suppose a nanometer-size sphere around each molecule, the local field contribution from its exterior is nearly equal to that from the continuum electrostatics and that from its interior yields the deviation from the classical Lorentz field. As a nonequilibrium problem, we investigate the dynamics after a reversal of applied field, where the relaxation is mostly caused by large-angle rotational jumps after 1 ps due to the presence of the hydrogen bond network. The molecules undergoing these jumps themselves form hydrogen-bonded clusters heterogeneously distributed in space.

cond-mat.soft↗

arXiv2013

Orientational glass in mixtures of elliptic and circular particles: Structural heterogeneities, rotational dynamics, and rheology

Using molecular dynamics simulation with an angle-dependent Lennard-Jones potential, we study orientational glass with quadrupolar symmetry in mixtures of elliptic particles and circular impurities in two dimensions. With a mild aspect ratio ($=1.2$) and a mild size ratio ($=1.2$), we realize a plastic crystal at relatively high temperature $T$. With further lowering $T$, we find a structural phase transition for very small impurity concentration $c$ and pinned disordered orientations for not small $c$. The ellipses are anchored by the impurities in the planar alignment. With increasing $c$, the orientation domains composed of isosceles triangles gradually become smaller, resulting in orientational glass with crystal order. In our simulation, the impurity distribution becomes heterogeneous during quenching from liquid, which then produces rotational dynamic heterogeneities. We also examine rheology in orientational glass to predict a shape memory effect and a superelasticity effect, where a large fraction of the strain is due to collective orientation changes.

cond-mat.soft↗

arXiv2013

Formation of double glass in binary mixtures of anisotropic particles: Dynamic heterogeneities in rotations and displacements

We study glass behavior in a mixture of elliptic and circular particles in two dimensions at low temperatures using an orientation-dependent Lennard-Jones potential. The ellipses have a mild aspect ratio ($\sim 1.2$) and tend to align at low temperatures, while the circular particles play the role of impurities disturbing the ellipse orientations at a concentration of 20%. These impurities have a size smaller than that of the ellipses and attract them in the homeotropic alignment. As a result, the coordination number around each impurity is mostly five or four in glassy states. We realize double glass, where both the orientations and the positions are disordered but still hold mesoscopic order. We find a strong heterogeneity in the flip motions of the ellipses, which sensitively depends on the impurity clustering. The average rotational diffusion constant is determined by rapidly flipping ellipses, which still remain even at low temperatures in our model. In contrast, the non-flip rotations (with angle changes not close to $\pm π$) are mainly caused by the cooperative configuration changes involving many particles. Then, there arises a long-time heterogeneity in the non-flip rotations closely correlated with the dynamic heterogeneity in displacements.

cond-mat.soft↗

arXiv2013

Applying electric field to charged and polar particles between metallic plates: Extension of the Ewald method

We develop an efficient Ewald method of molecular dynamics simulation for calculating the electrostatic interactions among charged and polar particles between parallel metallic plates, where we may apply an electric field with an arbitrary size. We use the fact that the potential from the surface charges is equivalent to the sum of those from image charges and dipoles located outside the cell. We present simulation results on boundary effects of charged and polar fluids, formation of ionic crystals, and formation of dipole chains, where the applied field and the image interaction are crucial. For polar fluids, we find a large deviation of the classical Lorentz-field relation between the local field and the applied field due to pair correlations along the applied field. As general aspects, we clarify the difference between the potential-fixed and the charge-fixed boundary conditions and examine the relationship between the discrete particle description and the continuum electrostatics.

cond-mat.soft↗

arXiv2013

Formation of double glass in binary mixtures of anisotropic particles

We study glass transitions in mixtures of elliptic and circular particles in two dimensions using an orientation-dependent Lennard-Jones potential. Changing anisotropic parameters of the potential, the size ratio, and the concentration, we realize double glass, where both the particle positions and orientations are disordered but still hold mesoscopic order. The ellipses are anchored around the circular impurities in the homeotropic or planar directions. We examine slowing-down of rotational and translational time-correlation functions. Turnover motions of the ellipses are activated more frequently than the configuration changes, where the latter cause the structural relaxation.

cond-mat.soft↗

arXiv2012

Molecular dynamics simulation of orientational glass formation in anisotropic particle systems in three dimensions

We propose a simple microscopic model of molecular dynamics simulation to study orientational glass in three dimensions. We present simulation results for mixtures of mildly anisotropic particles and spherical impurities. We realize fcc solids without orientational order in a rotator phase. As the temperature $T$ is lowered, the disordered matrix is gradually replaced by four kinds of orientationally ordered, rhombohedral domains. Two-phase coexistence is realized in a temperature window. The impurities serve to anchor the orientations of the surrounding anisotropic particles, resulting in finely divided domains or medium long-range orientational order. We examine the rotational dynamics of the molecular orientations which is slowed down at low $T$. We predict the shape memory effect under a stretching cycle due to inter-variant transformation.

cond-mat.soft↗