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The rotational dynamics of microparticles in liquids have a wide range of applications, including chemical microreactors, biotechnologies, microfluidic devices, tunable heat and mass transfer, and fundamental understanding of chiral active soft matter which refers to systems composed of particles that exhibit a handedness in their rotation, breaking mirror symmetry at the microscopic level. Here, we report on the study of two effects in colloids in rotating electric fields: (i) the rotation of individual colloidal particles in rotating electric field and related to that (ii) precession of pairs of particles. We show that the mechanism responsible for the rotation of individual particles is related to the time lag between the external field applied to the particle and the particle polarization. Using numerical simulations and experiments with silica particles in a water-based solvent, we prove that the observed rotation of particle pairs and triplets is governed by the tunable rotation of individual particles and can be explained and described by the action of hydrodynamic forces. Our findings demonstrate that colloidal suspensions in rotating electric fields, under some conditions, represent a novel class of chiral soft active matter-tunable colloidal spinners. The experiments and the corresponding theoretical framework we developed open novel prospects for future studies of these systems and for their potential applications., (© 2024 Author(s). Published under an exclusive license by AIP Publishing.)

Astrocytes are glycolytically active cells in the central nervous system playing a crucial role in various brain processes from homeostasis to neurotransmission. Astrocytes possess a complex branched morphology, frequently examined by fluorescent microscopy. However, staining and fixation may impact the properties of astrocytes, thereby affecting the accuracy of the experimental data of astrocytes dynamics and morphology. On the other hand, phase contrast microscopy can be used to study astrocytes morphology without affecting them, but the post-processing of the resulting low-contrast images is challenging. The main result of this work is a novel approach for recognition and morphological analysis of unstained astrocytes based on machine-learning recognition of microscopic images. We conducted a series of experiments involving the cultivation of isolated astrocytes from the rat brain cortex followed by microscopy. Using the proposed approach, we tracked the temporal evolution of the average total length of branches, branching, and area per astrocyte in our experiments. We believe that the proposed approach and the obtained experimental data will be of interest and benefit to the scientific communities in cell biology, biophysics, and machine learning., (© 2024. The Author(s).)

In vitro modeling of brain tissue is a promising but not yet resolved problem in modern neurobiology and neuropharmacology. Complexity of the brain structure and diversity of cell-to-cell communication in (patho)physiological conditions make this task almost unachievable. However, establishment of novel in vitro brain models would ultimately lead to better understanding of development-associated or experience-driven brain plasticity, designing efficient approaches to restore aberrant brain functioning. The main goal of this review is to summarize the available data on methodological approaches that are currently in use, and to identify the most prospective trends in development of neurovascular unit, blood-brain barrier, blood-cerebrospinal fluid barrier, and neurogenic niche in vitro models. The manuscript focuses on the regulation of adult neurogenesis, cerebral microcirculation and fluids dynamics that should be reproduced in the in vitro 4D models to mimic brain development and its alterations in brain pathology. We discuss approaches that are critical for studying brain plasticity, deciphering the individual person-specific trajectory of brain development and aging, and testing new drug candidates in the in vitro models., Competing Interests: The author(s) declared no potential conflicts of interest with respect to the research, authorship, and/or publication of this article., (© The Author(s) 2024.)

Swarming behavior in systems of self-propelled particles, whether biological or artificial, has received increased attention in recent years. Here, we show that even a small number of particles with anomalous behavior can change dramatically collective dynamics of the swarming system and can impose unusual behavior and transitions between dynamic states. Our results pave the way to practical approaches and concepts of multiagent dynamics in groups of flocking animals: birds, insects, and fish, i.e., active and living soft matter.

The effects of inertia in active matter and motility-induced phase separation (MIPS) have attracted growing interest but still remain poorly studied. We studied MIPS behavior in the Langevin dynamics across a broad range of particle activity and damping rate values with molecular dynamic simulations. Here we show that the MIPS stability region across particle activity values consists of several domains separated by discontinuous or sharp changes in susceptibility of mean kinetic energy. These domain boundaries have fingerprints in the system's kinetic energy fluctuations and characteristics of gas, liquid, and solid subphases, such as the number of particles, densities, or the power of energy release due to activity. The observed domain cascade is most stable at intermediate damping rates but loses its distinctness in the Brownian limit or vanishes along with phase separation at lower damping values.

Self-diffusion in fluids has been thoroughly studied numerically, but even for simple liquids just a few scaling relationships are known. Relations between diffusion, excitation spectra, and character of the interparticle interactions remain poorly understood. Here, we show that diffusion mobility of particles in simple fluids increases linearly on the liquid branch of the liquid-gas binodal, from the triple point almost up to the critical point. With molecular dynamics simulations, we considered bulk systems of particles interacting via a generalised Lennard-Jones potential, as well as ethane. Using a two-oscillator model for the analysis of excitations, we observed that the mobility (inverse diffusion) coefficient on the liquid-gas binodal increases linearly above the triple point until the dispersion of high-frequency spectra has a solid-like (oscillating) shape. In terms of a separate mode analysis (of longitudinal and transverse modes), this corresponds to crossed modes in the intermediate range of wavenumbers q, between the hydrodynamic regime (small q) and the regime of individual particle motion (large q). The results should be interesting for a broad community in physics and chemistry of fluids, since self-diffusion is among the most fundamental transport phenomena, important for prospective chemical technologies, micro-, nanofluidics, and biotechnologies., (© 2023. The Author(s).)

Coupled oscillators are one of the basic models in nonlinear dynamics. Here, we study numerically and analytically the spectra of two harmonic oscillators with stochastically fluctuating coupling and driving forces reproducing a thermostat. We show that, even at small coupling, vanishing on average, the oscillation spectra exhibit mixing, even though no cross-correlations exists between the oscillators. Our results reveal a new mechanism of mode mixing for stochastically uncorrelated systems that is crucial for analysis of spectra in various systems, from simple liquids to living systems.

Monolayer and two-dimensional (2D) systems exhibit rich phase behavior, compared with 3D systems, in particular, due to the hexatic phase playing a central role in melting scenarios. The attraction range is known to affect critical gas-liquid behavior (liquid-liquid in protein and colloidal systems), but the effect of attraction on melting in 2D systems remains unstudied systematically. Here, we have revealed how the attraction range affects the phase diagrams and melting scenarios in a 2D system. Using molecular dynamics simulations, we have considered the generalized Lennard-Jones system with a fixed repulsion branch and different power indices of attraction from long-range dipolar to short-range sticky-sphere-like. A drop in the attraction range has been found to reduce the temperature of the gas-liquid critical point, bringing it closer to the gas-liquid-solid triple point. At high temperatures, attraction does not affect the melting scenario that proceeds through the cascade of solid-hexatic (Berezinskii-Kosterlitz-Thouless) and hexatic-liquid (first-order) phase transitions. In the case of dipolar attraction, we have observed two triple points inherent in a 2D system: hexatic-liquid-gas and crystal-hexatic-gas, the temperature of the crystal-hexatic-gas triple point is below the hexatic-liquid-gas triple point. This observation may have far-reaching consequences for future studies, since phase diagrams determine possible routes of self-assembly in molecular, protein, and colloidal systems, whereas the attraction range can be adjusted with complex solvents and external electric or magnetic fields. The results obtained may be widely used in condensed matter, chemical physics, materials science, and soft matter.

Many-body forces play a prominent role in structure and dynamics of matter, but their role is not well understood in many cases due to experimental challenges. Here, we demonstrate that a novel experimental system based on rotating electric fields can be utilised to deliver unprecedented degree of control over many-body interactions between colloidal silica particles in water. We further show that we can decompose interparticle interactions explicitly into the leading terms and study their specific effects on phase behaviour. We found that three-body interactions exert critical influence over the phase diagram domain boundaries, including liquid-gas binodal, critical and triple points. Phase transitions are shown to be reversible and fully controlled by the magnitude of external rotating electric field governing the tunable interactions. Our results demonstrate that colloidal systems in rotating electric fields are a unique laboratory to study the role of many-body interactions in physics of phase transitions and in applications, such as self-assembly, offering exciting opportunities for studying generic phenomena inherent to liquids and solids, from atomic to protein and colloidal systems., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier Inc. All rights reserved.)

Among different thermodynamic properties of liquids, the entropy is one of the hardest quantities to estimate. Therefore, the development of models allowing accurate estimations of the entropy for different mechanisms of interatomic interactions represents an important problem. Here, we propose a method for estimating the excess entropy of simple liquids not too far from the liquid-solid phase transition. The method represents a variant of cell theory, which particularly emphasizes relations between liquid state thermodynamics and collective modes properties. The method is applied to calculate the excess entropy of inverse-power-law fluids with ∝r -n repulsive interactions. The covered range of potential softness is extremely wide, including the very soft Coulomb (n = 1) case, much steeper n = 6 and n = 12 cases, and the opposite hard-sphere interaction limit (n = ∞). An overall reasonably good agreement between the method's outcome and existing "exact" results is documented at sufficiently high fluid densities. Its applicability condition can be conveniently formulated in terms of the excess entropy itself. The method is also applied to the Lennard-Jones potential but demonstrates considerably lower accuracy in this case. Our results should be relevant to a broad range of liquid systems that can be described with isotropic repulsive interactions, including liquid metals, macromolecular systems, globular proteins, and colloidal suspensions.

Anisotropic particles are widely presented in nature, from colloidal to bacterial systems, and control over their interactions is of crucial importance for many applications, from self-assembly of novel materials to microfluidics. Placed in rapidly rotating external electric fields, colloidal particles attain a tunable long-range and many-body part in their interactions. For spherical colloids, this approach has been shown to offer rich capabilities to construct the tunable interactions via designing the internal structure of particles and spatial hodographs of external rotating fields, but in the case of anisotropic particles, the interactions remain poorly understood. Here, we show that tunable interactions between anisotropic rod-like and spheroidal colloidal particles in rotating electric or magnetic fields can be calculated and analyzed with the diagrammatic technique we developed in the present work. With this technique, we considered an in-plane rotating electric field, obtained the long-range asymptotics of the anisotropic interactions, calculated the tunable interactions between particles rotating synchronously, and found conditions for rotator repulsion. We compared the mechanisms providing tunable interactions to those for orientational (Keesom), induction (Debye), and dispersion (London) interactions in molecular systems and found that the tunable interactions between anisotropic particles represent a novel kind of dipole-like interaction. The method can be directly generalized for magnetically induced interactions, 3D systems, and fields with spatial hodographs. The results provide significant advance in theoretical methods for tunable interactions in colloids and, therefore, are of broad interest in condensed matter, chemical physics, physical chemistry, materials science, and soft matter.

Melting is one of the most studied phase transitions important for atomic, molecular, colloidal, and protein systems. However, there is currently no microscopic experimentally accessible criteria that can be used to reliably track a system evolution across the transition, while providing insights into melting nucleation and melting front evolution. To address this, we developed a theoretical mean-field framework with the normalised mean-square displacement between particles in neighbouring Voronoi cells serving as the local order parameter, measurable experimentally. We tested the framework in a number of colloidal and in silico particle-resolved experiments against systems with significantly different (Brownian and Newtonian) dynamic regimes and found that it provides excellent description of system evolution across melting point. This new approach suggests a broad scope for application in diverse areas of science from materials through to biology and beyond. Consequently, the results of this work provide a new guidance for nucleation theory of melting and are of broad interest in condensed matter, chemical physics, physical chemistry, materials science, and soft matter., (© 2021. The Author(s).)

Tunable interactions between colloidal particles, governed by external rotating electric or magnetic fields, yield rich capabilities for prospective self-assembly technologies of materials and fundamental particle-resolved studies of phase transitions and transport phenomena in soft matter. However, the role of the internal structure of colloidal particles in the tunable interactions has never been systematically investigated. Here, we study the tunable interactions between composite particles with core-shell structure in a rotating electric field and show that the engineering of their internal structure provides an effective tool for designing the interactions. We generalized an integral theory and studied the tunable interactions between core-shell particles with homogeneous cores (layered particles) and cores with nano-inclusions to reveal the main trends in the interactions influenced by the structure. We found that depending on the materials of the core, shell, and solvent, the interactions with the attractive pairwise part and positive or negative three-body part can be obtained, as well as pairwise repulsion with attractive three-body interactions (for triangular triplets). The latter case is observed for the first time, being unattainable for homogeneous particles but feasible with core-shell particles: Qualitatively similar interactions are inherent to charged colloids (repulsive pairwise and attractive three-body energies), known as a model system of globular proteins. The methods and conclusions of our paper can be generalized for magnetic and 3D colloidal systems. The results make a significant advance in the analysis of tunable interactions in colloidal systems, which are of broad interest in condensed matter, chemical physics, physical chemistry, materials science, and soft matter.

The effect of particle activity on collective excitations in active fluids of microflyers is studied. With an in silico study, we observed an oscillating breakdown of equipartition (uniform spectral distribution) of kinetic energy in reciprocal space. The phenomenon is related to short-range velocity-velocity correlations that were realized without forming of long-lived mesoscale vortices in the system. This stands in contrast to well-known mesoscale turbulence operating in active nematic systems (bacterial or artificial) and reveals the features of collective dynamics in active fluids, which should be important for structural transitions and glassy dynamics in active matter.

The conventional (Zwanzig-Mountain) expressions for instantaneous elastic moduli of simple fluids predict their divergence as the limit of hard-sphere (HS) interaction is approached. However, elastic moduli of a true HS fluid are finite. Here we demonstrate that this paradox reveals the soft-to-hard-sphere crossover in fluid excitations and thermodynamics. With extensive in silico study of fluids with repulsive power-law interactions (∝r^{-n}), we locate the crossover at n≃10-20 and develop a simple and accurate model for the HS regime. The results open prospects to deal with the elasticity and related phenomena in various systems, from simple fluids to melts and glasses.

The hydrogels of the polyelectrolytes polyethylenimine and poly(acrylic acid) are used to form a thin-layer interface on the gallium-indium eutectic alloy's surface. The proposed method of gradually increasing the applied voltage reveals the possibility of formation of electronic components: diode, capacitor, resistor, and memristor. The components can be changed to each other many times. A multilayer perceptron model with one hidden layer and 12 nodes allows identifying hydrogels' composition and automatically setting the desired architecture of electronic components. The design of electronic components makes it possible to easy-to-produce new electronic parts and programmable soft-matter electronics.

This work depicts an electrochemical hydrogel-eutectic gallium indium alloy interface for the detection of tick-borne encephalitis (TBE) virus. This interface allows recording of nonlinear current-voltage responses, depending on the composition of the hydrogel. The current-voltage data for the machine learning model are trained by a multilayer perceptron. This model accurately recognizes the TBE antibody, antigen, and an antibody-antigen complex in mixture with interfering bovine serum albumin with 93% accuracy. Thus, this interface can be used as a convenient method for expressed viruses and pathogens detection.

The change in dispersion of high-frequency excitations in fluids, from an oscillating solidlike to a monotonic gaslike one, is shown for the first time to affect thermal behavior of heat capacity and the q-gap width in reciprocal space. With in silico study of liquified noble gases, liquid iron, liquid mercury, and model fluids, we established universal bilinear dependence of heat capacity on q-gap width, whereas the crossover precisely corresponds to the change in the excitation spectra. The results open novel prospects for studies of various fluids, from simple to molecular liquids and melts.

Opening a way to designing tunable interactions between colloidal particles in rotating electric and magnetic fields provides rich opportunities both for fundamental studies of phase transitions and engineering of soft materials. Spatial hodographs, showing the distribution of the field magnitude and orientation, allow the adjustment of interactions and can be an extremely potent tool for prospective experiments, but remain unstudied systematically. Here, we calculate the tunable interactions between spherical particles in rhodonea, conical, cylindrical, and ellipsoidal field hodographs, as the most experimentally important cases. We discovered that spatial hodographs are reduced to each other, providing a plethora of interactions, e.g., repulsive, attractive, barrier-like, and double-scale repulsive ones. Complementing the "magic" conical angle, the "magic" compression and ellipticity of cylindrical and ellipsoidal hodographs are introduced. In the "magic" hodographs, the interactions become spatially isotropic and attain dispersion-force-like asymptotic (the same for pairwise and many-body energies), being attractive or repulsive, if the particle permittivity is larger or smaller than that of the solvent. With the diagrammatic method and numerical calculations, we obtained physically meaningful fits to the many-body tunable potentials for silica (iron oxide) particles in deionised water in the rotating electric (magnetic) fields. Our results provide essential guidance for future experiments and simulations of colloidal liquids, crystals, gels, and glasses, important for a broad range of problems in condensed matter, chemical physics, physical chemistry, materials science, and soft matter.

Newton's third law-the action-reaction symmetry-can be violated for effective interbody forces in open and nonequilibrium systems that are ubiquitous in areas as diverse as complex plasmas, colloidal suspensions, active and living soft matter, and social behavior. While studying monolayer complex plasma (confined charged particles in an ionized gas) with nonreciprocal interactions mediated by plasma flows, in silico we found that an interplay between melting and thermal activation drastically transforms the collective dynamics: the order-disorder transition modifies the system's thermal steady state so that the crystal tends to melt, whereas the fluid tends to freeze, jumping chaotically between the two states. We identified this collective chaotic behavior as strange attractors formed in a monolayer complex plasma and link the strange attractor behavior to the specifics of interparticle interactions.

A significant number of key properties of condensed matter are determined by the spectra of elementary excitations and, in particular, collective vibrations. However, the behavior and description of collective modes in disordered media (e.g., liquids and glasses) remains a challenging area of modern condensed matter science. Recently, anticrossing between longitudinal and transverse modes was predicted theoretically and observed in molecular dynamics simulations, but this fundamental phenomenon has never been observed experimentally. Here we demonstrate the mode anticrossing in a simple Yukawa fluid constructed from charged microparticles in weakly ionized gas. Theory, simulations, and experiments show clear evidence of mode anticrossing that is accompanied by mode hybridization and strong redistribution of the excitation spectra. Our results provide a significant advance in understanding excitations of fluids, opening new perspectives for studies of dynamics, thermodynamics, and transport phenomena in a wide variety of systems from noble-gas fluids and metallic melts to strongly coupled plasmas and molecular and complex fluids.

Tunable interactions in colloids, induced by rotating electric or magnetic fields, provide a flexible and promising tool for self-assembly of soft materials, as well as for fundamental particle-resolved studies of phase transitions and other generic phenomena in condensed matter. In the case of two-dimensional systems and the in-plane rotating fields, the interactions are known to have a long-range (dipolar) attraction and an expressed three-body part at short distances, but still remain poorly understood. Here, we show that the interactions and polarization mechanisms governing the tunable interactions can be described, calculated, and analyzed in detail with the diagrammatic method we proposed. The diagrams yield a clear illustration of different polarization processes contributing to the Keesom, Debye, London, self, and external energies, classified in colloids similarly to intermolecular interactions. The real tunable interactions, obtained with the boundary element method, can be simply and accurately interpolated with the set of basis of the diagrams attributed to different physically clear polarization processes. Calculation of large-distance behavior and interpolation of the many-body interactions (and analysis of the leading mechanisms contributing to them) excellently illustrate that the diagrammatic method provides deep insights into the nature of tunable interactions. The method can be generalized for multicomponent systems, suspensions of particles with a composite structure and a complicated shape. The results provide significant advance in theoretical methods for detailed analysis of tunable interactions in colloids and, therefore, the method is of broad interest in condensed matter, chemical physics, physical chemistry, materials science, and soft matter.

Accurate analysis of pair correlations in condensed matter allows us to establish relations between structures and thermodynamic properties and, thus, is of high importance for a wide range of systems, from solids to colloidal suspensions. Recently, the interpolation method (IM) that describes satisfactorily the shape of pair correlation peaks at short and at long distances has been elaborated theoretically and using molecular dynamics simulations, but it has not been verified experimentally as yet. Here, we test the IM by particle-resolved studies with colloidal suspensions and with complex (dusty) plasmas and demonstrate that, owing to its high accuracy, the IM can be used to experimentally measure parameters that describe interaction between particles in these systems. We used three- and two-dimensional colloidal crystals and monolayer complex (dusty) plasma crystals to explore suitability of the IM in systems with soft to hard-sphere-like repulsion between particles. In addition to the systems with pairwise interactions, if many-body interactions can be mapped to the pairwise ones with some effective (e.g., density-dependent) parameters, the IM could be used to obtain these parameters. The results reliably show that the IM can be effectively used for analysis of pair correlations and interactions in a wide variety of systems and therefore is of broad interest in condensed matter, complex plasma, chemical physics, physical chemistry, materials science, and soft matter.

Defects play a crucial role in physics of solids, affecting their mechanical, electromagnetic, and chemical properties. However, influence of thermal defects on wave propagation in exothermic reactions (flame fronts) still remains poorly understood at the molecular level. Here, we show that thermal behavior of the defects exhibits essential features of double-step exothermic reactions with preequilibrium. We use experiments with monolayer complex (dusty) plasma and find that it can show a double-step activation thermal behavior, similar to chemically reactive media. Furthermore, we demonstrate capabilities to control flame fronts using defects and the different dynamic regimes of the thermal defects in complex (dusty) plasmas, from a nonactivated one to being sound and self-activated (like in active soft matter). The results suggest that a range of challenging phenomena at the forefront of modern science (e.g., defect activation, flame front dynamics, reaction waves, etc.) can now be experimentally interrogated on a microscopic scale.

If interacting modes of the same symmetry cross, they repel from each other and become hybridized. This phenomenon is called anticrossing and is well-known for mechanical oscillations, electromagnetic circuits, waveguides, metamaterials, polaritons, and phonons in crystals, but it still remains poorly understood in simple fluids. Here, we show that structural disorder and anharmonicity, governing properties of fluids, lead to the anticrossing of longitudinal and transverse modes, which is accompanied by their hybridization and strong redistribution of excitation spectra. We combined theory and simulations for noble gases to prove the reliability of mode anticrossing in simple fluids, studied here for the first time. Our results open novel prospects in understanding collective dynamics, thermodynamics, and transport phenomena in various fluids, spanning from noble gas fluids and metallic melts to strongly coupled plasmas and molecular and complex fluids.

Although the understanding of excitation spectra in fluids is of great importance, it is still unclear how different methods of spectral analysis agree with each other and which of them is suitable in a wide range of parameters. Here, we show that the problem can be solved using a two-oscillator model to analyze total velocity current spectra, while other considered methods, including analysis of the spectral maxima and single mode analysis, yield rough results and become unsuitable at high temperatures and wavenumbers. To prove this, we perform molecular dynamics (MD) simulations and calculate excitation spectra in Lennard-Jones and inverse-power-law fluids at different temperatures, both in 3D and 2D cases. Then, we analyze relations between thermodynamic and dynamic features of fluids at (Frenkel) crossover from a liquid- to gas-like state and find that they agree with each other in the 3D case and strongly disagree in 2D systems due to enhanced anharmonicity effects. The results provide a significant advance in methods for detail analysis of collective fluid dynamics spanning fields from soft condensed matter to strongly coupled plasmas.

Adjustment of the environmental acidity is a powerful method for fine-tuning the outcome of many chemical processes. Numerous strategies have been developed for the modification of pH in bulk as well as locally. Electrochemical and photochemical processes provide a powerful approach for on-demand generation of ion concentration gradients locally at solid-liquid interfaces. Spatially organized in individual way electrodes provide a particular pattern of proton distribution in solution. It opens perspectives to iontronics which is a bioinspired approach to signaling, information processing, and storing by spatial and temporal distribution of ions. We prove here that soft layers allow to control of ion mobility over the surface as well as processes of self-organization are closely related to change in entropy. In this work, we summarize the achievements and discuss perspectives of ion gradients in solution for information processing.

A simple practical approach to describe transverse (shear) waves in strongly-coupled Yukawa fluids is presented. Theoretical dispersion curves, based on hydrodynamic consideration, are shown to compare favorably with existing numerical results for plasma-related systems in the long-wavelength regime. The existence of a minimum wave number below which shear waves cannot propagate and its magnitude are properly accounted in the approach. The relevance of the approach beyond plasma-related Yukawa fluids is demonstrated by using experimental data on transverse excitations in liquid metals Fe, Cu, and Zn, obtained from inelastic x-ray scattering. Some potentially important relations, scalings, and quasi-universalities are discussed. The results should be interesting for a broad community in chemical physics, materials physics, physics of fluids and glassy state, complex (dusty) plasmas, and soft matter.

We study the phase diagram of a two-dimensional (2D) system of colloidal particles, interacting via an isotropic potential with a short-ranged Yukawa repulsion and a long-ranged dipolar attraction. Such interactions in 2D colloidal suspensions can be induced by rapidly rotating in-plane magnetic (or electric) fields. Using computer simulations and liquid integral equation theory, we calculate the bulk phase diagram, which contains gas, crystalline, liquid, and supercritical fluid phases. The densities at the critical and triple points in the phase diagram are governed by the softness of Yukawa repulsion and can therefore be largely tuned. We observe that the liquid-gas binodals exhibit universal behavior when the effective temperature (given by the inverse magnitude of the dipolar attractions) is normalized by its value at the critical point and the density is normalized by the squared Barker-Henderson diameter. The results can be verified in particle-resolved experiments with colloidal suspensions.

The reciprocity of effective interparticle forces can be violated in various open and nonequilibrium systems, in particular, in colloidal suspensions and complex (dusty) plasmas. Here, we obtain a criterion under which a nonreciprocal system can be strictly reduced to a pseudo-Hamiltonian system with a detailed dynamic equilibrium. In particular, the criterion is satisfied for catalytically active colloids interacting via nonreciprocal diffusiophoretic forces. However, in the general case, when this criterion is not satisfied, the steady state is determined by the interplay between dissipation and the energy source due to the nonreciprocity of interactions. The results indicate the realization of bistability and dissipative spinodal decomposition in a broad class of systems with nonreciprocal effective interactions.

Tunable interactions between colloidal particles in external conically rotating electric fields are calculated, while the (vertical) axis of the field rotation is normal to the (horizontal) particle motion plane. The comparison of different approaches, including the methods of noninteracting, self-consistent dipoles, and the boundary element method, indicates that the last method is the most suitable for tunable interaction analysis. Thorough analysis, performed for interactions in pairs and clusters of colloidal particles, indicate that two- and three-body interactions make the main contributions in the interaction energy, while the effect of high-order terms is negligible. The tunable interactions are determined by the dielectric properties of the particles and solvent and can be changed in a wide range, providing a rich variety for the experimental "design" of different interactions, including repulsion, attraction, combination of short-range repulsion with long-range attraction, barrier-type interactions with short-range attraction and long-range repulsion, and double-scale repulsive (core-shoulder) interactions. These conclusions can be generalized for magnetically induced tunable interactions. The results indicate that tunable interactions can be widely applied in self-assembly and particle-resolved studies of generic phenomena in fluids and crystals, and, therefore, are of broad interest in the fields of chemical physics, physical chemistry, materials science, and soft matter.

Molecular dynamics simulations have been performed to investigate in detail collective modes spectra of two-dimensional Coulomb fluids in a wide range of coupling. The obtained dispersion relations are compared with theoretical approaches based on quasi-crystalline approximation, also known as the quasi-localized charge approximation, in the plasma-related context. An overall satisfactory agreement between theory and simulations is documented for the longitudinal mode at moderate coupling and in the long-wavelength domain at strong coupling. For the transverse mode, satisfactory agreement in the long-wavelength domain is only reached at very strong coupling, when the cutoff wave-number below which shear waves cannot propagate becomes small. The dependence of the cutoff wave-number for shear waves on the coupling parameter is obtained.

Thermoacoustic instability in a fluid monolayer complex plasma is studied for the first time. Experiments, theory, and simulations demonstrate that nonreciprocal effective interactions between particles (mediated by plasma flows) provide positive thermal feedback leading to acoustic sound amplification. The form of the generated sound spectra obtained both in experiments and simulations excellently agrees with theory, justifying thermoacoustic instability in the fluid complex plasma. The results indicate a physical analogy between collective fluctuation dynamics in reactive media and in systems with nonreciprocal effective interactions exposing an activation behavior.

The heat capacity of classical crystals is determined by the Dulong-Petit value C V ≃ D (where D is the spatial dimension) for softly interacting particles and has the gas-like value C V ≃ D/2 in the hard-sphere limit, while deviations are governed by the effects of anharmonicity. Soft- and hard-sphere interactions, which are associated with the enthalpy and entropy of crystals, are specifically anharmonic owing to violation of a linear relation between particle displacements and corresponding restoring forces. Here, we show that the interplay between these two types of anharmonicities unexpectedly induces two possible types of heat capacity anomalies. We studied thermodynamics, pair correlations, and collective excitations in 2D and 3D crystals of particles with a limited range of soft repulsions to prove the effect of interplay between the enthalpy and entropy types of anharmonicities. The observed anomalies are triggered by the density of the crystal, changing the interaction regime in the zero-temperature limit, and can provide about 10% excess of the heat capacity above the Dulong-Petit value. Our results facilitate understanding effects of complex anharmonicity in molecular and complex crystals and demonstrate the possibility of new effects due to the interplay between different types of anharmonicities.

A transition from a square to a hexagonal lattice is studied in a 2D system of particles interacting via a core-softened potential. Due to the presence of two length scales of repulsion, different local configurations with four, five, and six neighbors are possible, leading to the formation of complex crystals. The previously proposed interpolation method is generalized to calculate pair correlations in crystals whose unit cell consists of more than one particle. The high efficiency of the method is illustrated using a snub square lattice as a representative example. Molecular dynamics simulations show that the snub square lattice is broken upon heating, generating a high-density quasicrystalline phase with 12-fold symmetry (HD12 phase). A simple theoretical model is proposed to explain the physical mechanism responsible for this phenomenon: with an increase in the density (from square to hexagonal phases), the concentrations of different local configurations randomly realized through a plane tiling change, which minimizes the energy of the system. The calculated phase diagram in the intermediate density range justifies the existence of the HD12 phase and demonstrates a cascade of first-order transitions "square - HD12 - hexagonal" solid phases with increasing density. The results allow us to better understand the physical mechanisms responsible for the formation of quasicrystals, and, therefore, should be of interest for broad community in materials science and soft matter.

Thermodynamics and dynamics of a classical two-dimensional system with dipolelike isotropic repulsive interactions are studied systematically using extensive molecular dynamics (MD) simulations supplemented by appropriate theoretical approximations. This interaction potential, which decays as an inverse cube of the interparticle distance, belongs to the class of very soft long-ranged interactions. As a result, the investigated system exhibits certain universal properties that are also shared by other related soft-interacting particle systems (like, for instance, the one-component plasma and weakly screened Coulomb systems). These universalities are explored in this article to construct a simple and reliable description of the system thermodynamics. In particular, Helmholtz free energies of the fluid and solid phases are derived, from which the location of the fluid-solid coexistence is determined. The quasicrystalline approximation is applied to the description of collective modes in dipole fluids. Its simplification, previously validated on strongly coupled plasma fluids, is used to derive explicit analytic dispersion relations for the longitudinal and transverse wave modes, which compare satisfactory with those obtained from direct MD simulations in the long-wavelength regime. Sound velocities of the dipole fluids and solids are derived and analyzed.

Tunable interparticle interactions in colloidal suspensions are of great interest because of their fundamental and practical significance. In this paper we present a new experimental setup for self-assembly of colloidal particles in two-dimensional systems, where the interactions are controlled by external rotating electric fields. The maximal magnitude of the field in a suspension is 25 V/mm, the field homogeneity is better than 1% over the horizontal distance of 250 μm, and the rotation frequency is in the range of 40 Hz to 30 kHz. Based on numerical electrostatic calculations for the developed setup with eight planar electrodes, we found optimal experimental conditions and performed demonstration experiments with a suspension of 2.12 μm silica particles in water. Thanks to its technological flexibility, the setup is well suited for particle-resolved studies of fundamental generic phenomena occurring in classical liquids and solids, and therefore it should be of interest for a broad community of soft matter, photonics, and material science.

Thermodynamics of two-dimensional Yukawa (screened Coulomb or Debye-Hückel) systems is studied systematically using molecular dynamics (MD) simulations. Simulations cover very broad parameter range spanning from weakly coupled gaseous states to strongly coupled fluid and crystalline states. Important thermodynamic quantities, such as internal energy and pressure, are obtained and accurate physically motivated fits are proposed. This allows us to put forward simple practical expressions to describe thermodynamic properties of two-dimensional Yukawa systems. For crystals, in addition to numerical simulations, the recently developed shortest-graph interpolation method is applied to describe pair correlations and hence thermodynamic properties. It is shown that the finite-temperature effects can be accounted for by using simple correction of peaks in the pair correlation function. The corresponding correction coefficients are evaluated using MD simulation. The relevance of the obtained results in the context of colloidal systems, complex (dusty) plasmas, and ions absorbed to interfaces in electrolytes is pointed out.

In this paper, we introduce wide-aperture aspherical lens for high-resolution terahertz (THz) imaging. The lens has been designed and analyzed by numerical methods of geometrical optics and electrodynamics. It has been made of high-density polyethylene by shaping at computer-controlled lathe and characterized using a continuous-wave THz imaging setup based on a backward-wave oscillator and Golay detector. The concept of image contrast has been implemented to estimate image quality. According to the experimental data, the lens allows resolving two points spaced at 0.95λ distance with a contrast of 15%. To highlight high resolution in the THz images, the wide-aperture lens has been employed for studying printed electronic circuit board containing sub-wavelength-scale elements. The observed results justify the high efficiency of the proposed lens design.

Ion-stabilized nanobubbles in bulk aqueous solutions of various electrolytes were investigated. To understand the ion-specific mechanism of nanobubble stabilization, an approach based on the Poisson--Boltzmann equation at the nanobubble interface and in the near-surface layer was developed. It has been shown that the stabilization of nanobubbles is realized by the adsorption of chaotropic anions at the interface, whereas the influence of cosmotropic cations is weak. With increasing temperature, it should be accounted for by blurring the interface due to thermal fluctuations. As a result, the adsorbed state of ions becomes unstable: the nanobubble loses its stability and vanishes. This prediction was proven in our experiments. It turned out that in the case of liquid samples being kept in hermetically sealed ampules, where the phase equilibrium at the liquid-gas interface is fulfilled for any temperature, the volume number density of nanobubbles decreases with increasing temperature and this decrease is irreversible.

Effects of anharmonicity on the pair correlation function of classical crystals are studied. The recently proposed shortest-graph approach using the Gaussian representation of the individual correlation peaks (the peak width is determined by the length of the shortest graph connecting a given pair of particles) is further improved, to account for anharmonic corrections due to finite temperatures and hard-sphere-like interactions. Two major effects are identified, leading to a modification of the correlation peaks at large or short distances: (i) the peaks at large distances, well described by Gaussians, should be calculated from the finite-temperature phonon spectra; (ii) at short distances, the correlation peaks deviate significantly from the Gaussian form due to the lattice discreteness. We propose the analytical interpolation method, based on the shortest-graph approach, which includes both effects. By employing the molecular dynamics simulations, the accuracy of the method is verified for three- and two-dimensional crystals with the Yukawa, inverse-power-law, and pseudo-hard-sphere pair interactions. The capabilities of the method are demonstrated by calculating the phase diagram of a three-dimensional Yukawa system.

A hybrid (active-passive mode) terahertz (THz) imaging system and an algorithm for imaging synthesis are proposed to enhance the THz image quality. The concept of image contrast is used to compare active and passive THz imaging. Combining the measurement of the self-emitted radiation of the object with the back-scattered source radiation measurement, it becomes possible to use the THz image to retrieve maximum information about the object. The experimental results confirm the advantages of hybrid THz imaging systems, which can be generalized for a wide range of applications in the material sciences, chemical physics, bio-systems, etc.

The shortest-graph method is applied to calculate the pair correlation functions of crystals. The method is based on the representation of individual correlation peaks by the Gaussian functions, summed along the shortest graph connecting the two given points. The analytical expressions for the Gaussian parameters are derived for two- and three-dimensional crystals. The obtained results are compared with the pair correlation functions deduced from the molecular dynamics simulations of Yukawa, inverse-power law, Weeks-Chandler-Andersen, and Lennard-Jones crystals. By calculating the Helmholtz free energy, it is shown that the method is particularly accurate for soft interparticle interactions and for low temperatures, i.e., when the anharmonicity effects are insignificant. The accuracy of the method is further demonstrated by deriving the solid-solid transition line for Yukawa crystals, and the compressibility for inverse-power law crystals.

Simple practical approach to estimate thermodynamic properties of strongly coupled Yukawa systems, in both fluid and solid phases, is presented. The accuracy of the approach is tested by extensive comparison with direct computer simulation results (for fluids and solids) and the recently proposed shortest-graph method (for solids). Possible applications to other systems of softly repulsive particles are briefly discussed.

A new method for approximate calculation of the pair correlation function g(r) is proposed for crystalline systems of identical particles with isotropic interactions. The main idea of the method is to account for the relative delocalization of each node in g(r) by using only the shortest lattice graph between the given points, thus neglecting smaller contributions from other (non-shortest) graphs. By employing the Lennard-Jones and Yukawa crystalline systems as representative examples, it is shown that the proposed approach yields very good agreement with the results of molecular dynamics simulations up to the melting line. The approach can be useful in approximating the structure of simple crystals (in particular, of crystalline colloids and plasma crystals), and can also be generalized for systems with anisotropic interactions.

A qualitative model of the nucleation of stable bubbles in water at room temperature is suggested. This model is completely based on the property of the affinity of water at the nanometer scale; it is shown that under certain conditions the extent of disorder in a liquid starts growing, which results in a spontaneous decrease of the local density of the liquid and in the formation of nanometer-sized voids. These voids can serve as nuclei for the following generation of the so-called bubstons (the abbreviation for bubbles, stabilized by ions). The model of charging the bubstons by the ions, which are capable of adsorption, and the screening by a cloud of counter-ions, which are incapable of adsorption, is analyzed. It was shown that, subject to the charge of bubston, two regimes of such screening can be realized. At low charge of bubston the screening is described in the framework of the known linearized Debye-Huckel approach, when the sign of the counter-ion cloud preserves its sign everywhere in the liquid surrounding the bubston, whereas at large charge this sign is changed at some distance from the bubston surface. This effect provides the mechanism of the emergence of two types of compound particles having the opposite polarity, which leads to the aggregation of such compound particles by a ballistic kinetics.