Coffee-ring formation through the use of the multi-ring mechanism guided by the self-assembly of magnetic nanoparticles.

The control of the mechanism leading to the appearance of the ring-shaped stains from the dried liquid colloidal droplets has been the subject of intense studies over the last 25 years. This stems from the immense significance of this effect for technological applications. One of the key open topics in this field is the emergence of a regular multi-ring deposit from the dried droplet. Here, we show that magnetic nanoparticles in a drying magnetic liquid droplet can self-assemble into a multi-ring deposit structure, and even more importantly, a magnetic field can be turned on to control the underlying processes. The magnetic liquid is prepared as an aqueous suspension of Fe[Formula: see text]O[Formula: see text] magnetic nanoparticles stabilized with (3-Aminopropyl)triethoxysilane (APTES) and its droplets are placed on low-density polyethylene (LDPE) film. The results of this work are expected to be very promising in the case of multiple applications including ink-jet printing methods and 2D printed electronics.

Kinetic Monte Carlo simulations of proton conductivity.

The kinetic Monte Carlo method is used to model the dynamic properties of proton diffusion in anhydrous proton conductors. The results have been discussed with reference to a two-step process called the Grotthuss mechanism. There is a widespread belief that this mechanism is responsible for fast proton mobility. We showed in detail that the relative frequency of reorientation and diffusion processes is crucial for the conductivity. Moreover, the current dependence on proton concentration has been analyzed. In order to test our microscopic model the proton transport in polymer electrolyte membranes based on benzimidazole C(7)H(6)N(2) molecules is studied.

Critical Casimir forces along the isofields.

Using quasiexact numerical density-matrix renormalization-group techniques we calculate the critical Casimir force for a two-dimensional (2D) Ising strip with equal strong surface fields, along the thermodynamic paths corresponding to the fixed nonzero bulk field h≠0. Using the Derjaguin approximation we also determine the critical Casimir force and its potential for two disks. We find that varying the temperature along the isofields lying between the bulk coexistence and the capillary condensation critical point leads to a dramatic increase of the critical Casimir interactions with a qualitatively different functional dependence on the temperature than along h=0. These findings might be of relevance for biomembranes, whose heterogeneity is recently interpreted as being connected with a critical behavior belonging to the 2D Ising universality class.

Translocation of polymers in a lattice model.

Voltage-driven polymer translocation is studied by means of a stochastic lattice model. The model incorporates voltage drop over the membrane as a bias in the hopping rate through the pore and exhibits the two main ingredients of the translocation process: driven motion through the pore and diffusive supply of chain length towards the pore on the cis-side and the drift away from the pore on the trans-side. The translocation time is either bias limited or diffusion limited. In the bias-limited regime the translocation time is inversely proportional to the voltage drop over the membrane. In the diffusion-limited regime the translocation time is independent of the applied voltage, but it is rather sensitive to the motion rules of the model. We find that the whole regime is well described by a single curve determined by the initial slope and the saturation value. The dependence of these parameters on the length of the chain, the motion rules and the repton statistics are established. Repulsion of reptons as well as the increase of chain length decrease the throughput of the polymer through the pore. As for free polymers, the inclusion of a mechanism for hernia creations/annihilations leads to the cross-over from Rouse-like behaviour to reptation. For the experimentally most relevant case (Rouse dynamics) the bimodal power law dependence of the translocation time on the chain length is found.

Capillary condensation in a square geometry with surface fields.

We study the influence of wetting on capillary condensation for a simple fluid in a square geometry with surface fields, where the reference system is an infinitely long slit. The corner transfer matrix renormalization group method has been extended to study a two-dimensional Ising model confined in an L × L geometry with equal surface fields. Our results have confirmed that in both geometries the coexistence line shift is governed by the same scaling powers, but their prefactors are different.

Critical wetting transitions in two-dimensional systems subject to long-ranged boundary fields.

Using the quasiexact density-matrix renormalization-group method and ground-state analysis we study interface delocalization transitions in wide two-dimensional Ising strips subject to long-ranged boundary fields with opposite signs at the two surfaces. Based on this approach, our explicit calculations demonstrate that critical wetting transitions do exist for semi-infinite two-dimensional systems even if the corresponding effective interface potentials decay asymptotically for large l as slow as l(-delta) with delta<2, where l is the distance of the mean interface position from the one-dimensional surface. This supersedes opposite claims by Kroll and Lipowsky [Phys. Rev. B 28, 5273 (1983)] and by Privman and Svrakic [Phys. Rev. B 37, 5974 (1988)] obtained within effective interface models. The corresponding wetting phase diagram is determined, including the cases delta=2 and delta=49 with the latter mimicking short-ranged surface fields. Our analysis highlights the limits of reliability of effective interface models.

Interplay of complete wetting, critical adsorption, and capillary condensation.

The excess adsorption Gamma in two-dimensional Ising strips (infinityxL), subject to identical boundary fields at both one-dimensional surfaces decaying in the orthogonal direction j as -h1j(-p), is studied for various values of p and along various thermodynamic paths below the bulk critical point by means of the density-matrix renormalization-group method. The crossover behavior between the complete-wetting and critical-adsorption regimes, occurring in semi-infinite systems, is strongly influenced by confinement effects. Along isotherms T=const the asymptotic power-law dependences on the external bulk field, which characterize these two regimes, are pre-empted by capillary condensation. Along the pseudo-first-order phase-coexistence line of the strips, which varies with temperature, we find a broad crossover regime in which both the thickness of the wetting film and Gamma increase as functions of the reduced temperature tau but do not follow any power law. Above the wetting temperature the order-parameter profiles are not slablike but exhibit wide interfacial variations and pronounced tails.

Tests of nonuniversality and finite-size scaling for two-dimensional wetting with long-ranged forces.

Effective Hamiltonian models predict nonuniversal critical singularities for two-dimensional wetting transitions with marginal long-ranged forces. We test these predictions by studying interfacial delocalization transitions in an infinitely long Ising strip, of width L (lattice spacings), with external fields that are long ranged and have opposite signs at each surface. Finite-size scaling suggests that the shift of the delocalization temperature T(c)(L) below the (semi-infinite) wetting temperature T(w) scales as L(-1/beta(s)) with beta(s) the adsorption critical exponent. Density-matrix renormalization-group methods allow us to study the behavior of T(c)(L) for L up to several hundred lattice spacings. For short-ranged forces the method recovers the universal value of beta(s)=1 known from the exact solution. While marginal long-ranged forces strongly influence the finite-size scaling of T(c)(L) , the extrapolated asymptotic value for the exponent beta(s) does not appear to confirm the predicted nonuniversality, but instead approaches the same universal value representative of systems with short-ranged forces.

Crossover from reptation to Rouse dynamics in the cage model.

The two-dimensional cage model for polymer motion is discussed with an emphasis on the effect of sideways motions, which cross the barriers imposed by the lattice. Using the density matrix method as a solver of the master equation, the renewal time and the diffusion coefficient are calculated as a function of the strength of the barrier crossings. A strong crossover influence of the barrier crossings is found and it is analyzed in terms of effective exponents for a given chain length. The crossover scaling functions and the crossover scaling exponents are calculated.

Solvation force for long-ranged wall--fluid potentials.

The solvation force of a simple fluid confined between identical planar walls is studied in two model systems with short ranged fluid-fluid interactions and long-ranged wall-fluid potentials decaying as -Az(-p),z--> infinity, for various values of p. Results for the Ising spins system are obtained in two dimensions at vanishing bulk magnetic field h=0 by means of the density-matrix renormalization-group method; results for the truncated Lennard-Jones (LJ) fluid are obtained within the nonlocal density functional theory. At low temperatures the solvation force f(solv) for the Ising film is repulsive and decays for large wall separations L in the same fashion as the boundary field f(solv) approximately L(-p), whereas for temperatures larger than the bulk critical temperature f(solv) is attractive and the asymptotic decay is f(solv) approximately L(-(p+1)). For the LJ fluid system f(solv) is always repulsive away from the critical region and decays for large L with the the same power law as the wall-fluid potential. We discuss the influence of the critical Casimir effect and of capillary condensation on the behavior of the solvation force.

Pulling reptating polymers by one end: magnetophoresis in the Rubinstein-Duke model.

We consider the magnetophoresis problem within the Rubinstein-Duke model, i.e., a reptating polymer pulled by a constant field applied to a single end of a chain. Extensive density matrix renormalization calculations are presented of the drift velocity and the profile of the chain for various strengths of the driving field and chain lengths. We show that the velocities and the average densities of the stored length are well described by simple interpolating crossover formulas, derived under the assumption that the difference between the drift and curvilinear velocities vanishes for sufficiently long chains. The profiles, which describe the average shape of the reptating chain, also show such interesting features as some nonmonotonic behavior of the link densities for sufficiently strong pulling fields. We develop a description in which a distinction is made between links entering at the pulled head and at the unpulled tail. At weak fields the separation between the head zone and the tail zone meanders through the whole chain, while the probability of finding it close to the edges drops off. At strong fields the tail zone is confined to a small region close to the unpulled edge of the polymer.

Near-critical confined fluids and Ising films: density-matrix renormalization-group study.

Two-dimensional Ising strips subject to identical surface fields h(1)=h(2) > or =0 are studied for temperatures above and below the bulk critical temperature T(c) and a range of bulk fields h by means of the density-matrix renormalization-group method. In the case of nonvanishing surface fields, the near-critical behavior of the solvation force f(solv), total adsorption Gamma, inverse longitudinal correlation length xi(parallel)( -1) and specific heat C(H) is strongly influenced by the (pseudo) capillary condensation that occurs below T(c). We obtain scaling functions of f(solv), Gamma, and xi(parallel)(-1). C(H) exhibits a weakly rounded singularity on crossing the pseudocoexistence line. We contrast these results with those for the case of free boundaries where, for temperatures slightly below T(c), f(solv) and C(H) exhibit a sharp extremum away from h=0. Our results have direct repercussions for the properties of near-critical Ising films in three dimensions and we argue that the long-ranged solvation (Casimir) force in confined fluids should be more attractive in the neighborhood of the capillary critical point than exactly at the bulk critical point.

Universal phase boundary shifts for corner wetting and filling.

The phase boundaries for corner wetting (filling) in square and diagonal lattice Ising models are exactly determined and show a universal shift relative to wetting near the bulk criticality. More generally, scaling theory predicts that the filling phase boundary shift for wedges and cones is determined by a universal scaling function R(d)(psi) depending only on the opening angle 2psi. R(d)(psi) is determined exactly in d = 2 and approximately in higher dimensions using nonclassical local functional and mean-field theory. Detailed numerical transfer matrix studies of the magnetization profile in finite-size Ising squares support the conjectured connection between filling and the strong-fluctuation regime of wetting.

Crossover between ordinary and normal transitions in the presence of a bulk field.

We investigate two-dimensional Ising films at the critical temperature T(c) and nonzero bulk magnetic field h using the density-matrix renormalization-group method. The crossover between ordinary (h(1)=0) and normal (h(1)=infinity) transitions corresponding to finite values of the surface fields h(1)=h(2), is studied. The structure and the solvation force f(solv) as a function of h, crucially depend on the value of h(1). Scaling functions for f(solv) and the longitudinal correlation length are given and discussed.

Crossover behavior for long reptating polymers.

The Rubinstein-Duke model for polymer reptation is analyzed by means of density matrix renormalization techniques. It is found that the crossover in the scaling behavior of polymer renewal time (or viscosity) arises from the competing effect of the contribution due to tube length fluctuations and higher-order corrections, which are of opposite sign. Experiments which ought to emphasize both contributions are suggested. The exponent describing the subleading scaling behavior of the diffusion coefficient is also investigated.

Coexistence of excited states in confined ising systems

Using the density-matrix renormalization-group method we study the two-dimensional Ising model in an infinite strip geometry with free-boundary conditions. The renormalization scheme enables us to consider systems of width up to 300 (lattice spacings) and study the influence of the bulk magnetic field on correlation function structure for all temperatures. From our numerical results we have determined the crossover line for the correlation length related to the coexistence of the excited states. A detailed scaling study of this line is performed. Our numerical results support and further specify previous conclusions reached by Abraham, Parry, and Upton based on the bubble model of correlations.

Cumulant ratios and their scaling functions for ising systems in a strip geometry

We calculate the fourth-order cumulant ratio (proposed by Binder) for the two-dimensional Ising model in the strip geometry Lxinfinity. The density-matrix renormalization-group method enables us to consider typical open boundary conditions up to L=200. Universal scaling functions of the cumulant ratio are determined for strips with parallel as well as opposing surface fields. Their asymptotic properties are also examined.

Influence of capillary condensation on the near-critical solvation force.

We argue that in a fluid, or magnet, confined by adsorbing walls which favor liquid, or the (+) phase, the solvation (Casimir) force in the vicinity of the critical point is strongly influenced by capillary condensation which occurs below the bulk critical temperature T(c). At T slightly below and above T(c), a small bulk field h<0, which favors gas, or the (-) phase, leads to residual condensation and a solvation force which is much more attractive (at the same large wall separation) than that found exactly at the critical point. Our predictions are supported by results obtained from density-matrix renormalization-group calculations in a two-dimensional Ising strip subject to identical surface fields.

Effect of bulk magnetic field on critical Ising films

Two-dimensional Ising films L x infinity in a nonvanishing bulk magnetic field H are studied at the bulk critical temperature Tc for two choices of surface fields (a) H1 = HL = 0 (ordinary transition), and (b) H1 = HL = infinity (normal transition) by the density-matrix renormalization-group method. Universal scaling functions for magnetization profiles, the excess magnetization gamma, the longitudinal correlation length xi parallel, and for the analog of the solvation force fsolv are found and discussed. When H1 = 0 the scaling function for fsolv has two symmetric minima at y = sgn(H)L magnitude of H nu/delta approximately +/- 1 with an amplitude at the minimum about 3.8 times the value at H = 0, the Casimir amplitude. For the normal transition the scaling function for fsolv has a single minimum near the continuation of the pseudocoexistence (capillary condensation) line, with an amplitude about 100 times the Casimir amplitude.

Crossover between ordinary and normal transitions in two dimensional critical Ising films.

We investigate two dimensional critical Ising films of width L with surface fields H(1)=H(L) in the crossover between ordinary (H(1)=0) and normal (H(1)=infinity) transitions. Using exact transfer-matrix diagonalization and density matrix renormalization-group (DMRG) methods, we calculate magnetization profiles m(z), the excess magnetization Gamma, and the analog of the solvation force f(solv) as functions of H1 for several L. Scaling functions of the above quantities deviate substantially from their asymptotic forms at fixed points for a broad region of the scaling variable LH21 approximately L/l(1), where l(1) is the length induced by the surface field H1. The scaling function for /f(solv)/ has a deep minimum near LH(2)(1)=1, which is about one order of magnitude smaller than its value at both fixed points (the "Casimir" amplitude). For weak H1 (l(1)>L) the magnetization profile has a maximum at the center of the film, and f(solv) decays much faster than L-2. For stronger H1 (1>l(1) the solvation force decays according to the universal power law f(solv) approximately L(-2). The results of the approximate DMRG method show remarkable agreement with the exact ones.