We re-examine the ordering behavior of a one-dimensional fluid of freely rotating hard needles, where the centers of mass of the particles are restricted to a line. Analytical equations are obtained for the equation of state, order parameter and orientational correlation functions using the transfer-matrix method if some simplifying assumptions are applied for either the orientational freedom or the contact distance between two needles. The two-state Zwanzig model accounts for the orientational ordering, but it produces unphysical pressure at high densities and there is no orientational correlation. The four-state Zwanzig model gives reasonable results for orientational correlation function, but the pressure is still poorly represented at high densities. In the continuum limit, apart from the orientational correlation length it is managed to reproduce all relevant bulk properties of the hard needles using an approximate formula for the contact distance. The results show that the orientational correlation length diverges at zero and infinite pressures. The high density behavior of needles is not resolved.
We study a one dimensional gas of needle-like objects as a testing ground for a formalism that relates the thermodynamic properties of "hard" potentials to the probabilities for contacts between particles. Specifically, we use Monte Carlo methods to calculate the pressure and elasticity coefficient of the hard-needle gas as a function of its density. The results are then compared to the same quantities obtained analytically from a transfer matrix approach.
We perform extensive Monte Carlo simulations of a two-dimensional bent hard-needle model in both its chiral zig-zag and its achiral bow-shape configurations and present their phase diagrams. We find evidence for a variety of stable phases: isotropic, quasi-nematic, smectic-C, anti-ferromorphic smectic-A, and modulated-nematic. This last phase consists of layers formed by supramolecular arches. They create a periodic modulation of the molecular polarity whose period is sensitively controlled by molecular geometry. We identify transition densities using correlation functions together with approp…
We consider a ternary mixture of hard colloidal spheres, ideal polymer spheres, and rigid vanishingly thin needles, which model stretched polymers or colloidal rods. For this model we develop a geometry-based density functional theory, apply it to bulk fluid phases, and predict demixing phase behavior. In the case of no polymer-needle interactions, two-phase coexistence between colloid-rich and -poor phases is found. For hard needle-polymer interactions we predict rich phase diagrams, exhibiting three-phase coexistence, and reentrant demixing behavior.
We have developed a kinetic theory of hard needles undergoing binary collisions with loss of energy due to normal and tangential restitution. In addition, we have simulated many particle systems of granular hard needles. The theory, based on the assumption of a homogeneous cooling state, predicts that granular cooling of the needles proceeds in two stages: An exponential decay of the initial configuration to a state where translational and rotational energies take on a time independent ratio (not necessarily unity), followed by an algebraic decay of the total kinetic energy $\sim t^{-2}$. The …
The transport of an infinitely thin, hard rod in a random, dense array of point obstacles is investigated by molecular dynamics simulations. Our model mimics the sterically hindered dynamics in dense needle liquids. The center-of-mass diffusion exhibits a minimum, and transport becomes increasingly fast at higher densities. The diffusion coefficient diverges according to a power law in the density with an approximate exponent of 0.8. This observation is connected with a new divergent time scale, reflected in a zig-zag motion of the needle, a two-step decay of the velocity-autocorrelation funct…
The isotropic-to-nematic transition in a two-dimensional fluid of hard needles is studied using grand canonical Monte Carlo simulations, multiple histogram reweighting, and finite size scaling. The transition is shown to be of the Kosterlitz-Thouless type, via a direct measurement of the critical exponents eta and beta, of the susceptibility and order parameter, respectively. At the transition, eta=1/4 and beta=1/8 are observed, in excellent agreement with Kosterlitz-Thouless theory. Also the shift in the chemical potential of the nematic susceptibility maximum with system size is in good agre…
Deposition and evaporation of infinitely thin hard rods (needles) is studied in two dimensions using Monte Carlo simulations. The ratio of deposition to evaporation rates controls the equilibrium density of rods, and increasing it leads to an entropy-driven transition to a nematic phase in which both static and dynamical orientational correlation functions decay as power laws, with exponents varying continuously with deposition-evaporation rate ratio. Our results for the onset of the power-law phase agree with those for a conserved number of rods. At a coarse-grained level, the dynamics of the…
We investigate the early part of the crystal nucleation process in the hard sphere fluid using data produced by computer simulation. We find that hexagonal order manifests continuously in the overcompressed liquid, beginning approximately one diffusion time before the appearance of the first `solid-like' particle of the nucleating cluster, and that a collective influx of particles towards the nucleation site occurs simultaneously to the ordering process: the density increases leading to nucleation are generated by the same individual particle displacements as the increases in order. We rule ou…
The phase behaviour and structural properties of a monolayer of hard particles is examined in such a confinement, where the adsorbed particles are constrained to the surface of a narrow hard cylindrical pore. The diameter of the pore is chosen such that only first and second neighbour interactions occur between the hard particles. The transfer operator method of Percus and Zhang [Mol. Phys., 69, 347 (1990)] is reformulated to obtain information about the structure of the monolayer. We have found that a true phase transition is not possible in the examined range of pore diameters. The monolayer…
In this article we calculate the surface phase diagram of a two-dimensional hard-rod fluid confined between two hard lines. In a first stage we study the semi-infinite system consisting of an isotropic fluid in contact with a single hard line. We have found complete wetting by the columnar phase at the wall-isotropic fluid interface. When the fluid is confined between two hard walls, capillary columnar ordering occurs via a first-order phase transition. For higher chemical potentials the system exhibits layering transitions even for very narrow slits (near the one-dimensional limit). The theor…
We study an experimental system of hard granular squares in two dimensions, energized by vibration. The interplay of order in the orientations and positions of anisotropic particles allows for a rich set of phases. We measure the structure and dynamics of steady states as a function of particle density. This allows us to identify a progression of phases in which a low density isotropic fluid gives way to a phase with tetratic orientational order, short-range translational correlations, and slowed rotational dynamics. In this range of density we also observe a coupling between the molecular ori…
Orientational ordering and close packing properties of quasi-one-dimensional hard Gaussian overlap particles
Institute for Applied Physics, University of Tübingen（蒂宾根大学应用物理研究所）；Physics Department, Centre for Natural Sciences, University of Pannonia（佩奇大学自然科学中心物理系）
Using Density Functional Theory we theoretically study the orientational properties of uniform phases of hard kites -- two isosceles triangles joined by their common base. Two approximations are used: Scaled Particle Theory, and a new approach which better approximates third virial coefficients of two-dimensional hard particles. By varying some of their geometrical parameters kites can be transformed into squares, rhombuses, triangles, and also very elongated particles, even reaching the hard-needle limit. Thus a fluid of hard kites, depending on the particle shape, can stabilize isotropic, ne…
We consider a Jepsen gas of $N$ hard-point particles undergoing free expansion on a line, starting from random initial positions of the particles having random initial velocities. The particles undergo binary elastic collisions upon contact and move freely in-between collisions. After a certain ordering time $T_{o}$, the system reaches a ``fan'' state where all the velocities are completely ordered from left to right in an increasing fashion and there is no further collision. We compute analytically the distributions of (i) the total number of collisions and (ii) the ordering time $T_{o}$. We …
Using scaled-particle theory for binary mixtures of two-dimensional hard particles with rotational freedom, we analyse the stability of nematic phases and the demixing phase behaviour of a variety of mixtures, focussing on cases where at least one of the components consists of hard rectangles or hard squares. A pure fluid of hard rectangles may exhibit, aside from the usual uniaxial nematic phase, an additional (tetratic) oriented phase, possessing two directors, which is the analogue of the biaxial or cubatic phases in three- dimensional fluids. There is computer simulation evidence that the …
We investigate the effect of three-body correlations on the phase behavior of hard rectangle two-dimensional fluids. The third virial coefficient, $B_3$, is incorporated via an equation of state that recovers scaled particle theory for parallel hard rectangles. This coefficient, a functional of the orientational distribution function, is calculated by Monte Carlo integration, using an accurate parameterized distribution function, for various particle aspect ratios in the range 1-25. A bifurcation analysis of the free energy calculated from the obtained equation of state is applied to find the …
We apply a recently proposed density functional for mixtures of parallel hard cylinders, based on Rosenfeld's fundamental measure theory, to study the effect of length-polydispersity on the relative stability between the smectic and columnar liquid crystal phases.To this purpose we derive from this functional an expression for the direct correlation function and use it to perform a bifurcation analysis. We compare the results with those obtained with a second and a third virial approximation of this function. All three approximations lead to the same conclusion: there is a terminal polydispers…
We study thermodynamics properties of a one dimensional gas of hard elongated particles. The particle centers are restricted to a line, while they can rotate in two-dimensional space. Correlations between orientations of the objects are studied (by transfer matrix method) as a function of density and aspect ratio. The behavior in the extreme high-density (jamming) limit is described by a few universality classes depending on the object's shape. In particular, there is a diverging correlation length when the contact point of adjacent objects is far from the line along which their centers move, …
The available virial coefficients for the 2D hard disks model are transformed into a matrix representation of the thermodynamic potentials, which allows for an accurate description of the whole fluid phase, up to the phase transition. We find that the fluid phase terminates at the transition point, supporting the Kosterlitz-Thouless-Halperin-Nelson-Young picture of a second order phase transition into a Hexatic phase. The density and pressure at the transition are calculated from the available first ten virial coefficients, and are found to be in excellent agreement with recent Monte-Carlo cal…
Using an extension of Pirogov-Sinai theory we prove phase transitions, corresponding to sublattice orderings, for a general class of hard core lattice particle systems with a finite number of close packed configurations. These include many cases for which such transitions have been proven. The proof also shows that, for these systems, the Gaunt-Fisher expansion of the pressure in powers of the inverse fugacity (aside from an explicit logarithmic term) has a nonzero radius of convergence.
We examine a two-dimensional nonequilibrium lattice model where particles adsorb at empty sites and desorb when the number of neighbouring particles is greater than a given threshold. In a certain range of parameters the model exhibits entropic ordering similar to some hard-core systems. However, contrary to hard-core systems, upon increasing the density of particles the ordering gets destroyed. In the heterogenous version of our model a regime with slow dynamics appears, that might indicate formation of some kind of glassy structures.
For hard ellipsoids of revolution we calculate the phase diagram for the idealized glass transition. Our equations cover the glass physics in the full phase space, for all packing fractions and all aspect ratios X$_0$. With increasing aspect ratio we find the idealized glass transition to become primarily be driven by orientational degrees of freedom. For needle or plate like systems the transition is strongly influenced by a precursor of a nematic instability. We obtain three types of glass transition lines. The first one ($ϕ_c^{(B)}$) corresponds to the conventional glass transition for sphe…
We calculate a collective number of thermodynamic quantities in a one-dimensional gas of hard elongated objects (such as needles) whose centers mobile on a line. Our formalism uses an approximation for the probabilities of contact between the objects. We show that in moderate pressures the quantities extracted from the noncentral potential do not rely on its noncentrality, instead we can extract them analytically from a central potential. Our formalism reproduces the nontrivial features of a gas of elongated objects. Finally, we show below a crossover pressure $p_o$ the rotational couplings ca…
We report two phenomena, induced by dynamical correlations, that occur during the free cooling of a two-dimensional mixture of inelastic hard disks. First, we show that, due to the onset of velocity correlations, the ratio of the kinetic energies associated with the two species changes from the value corresponding to the homogeneous cooling state to a value approximately given by the mass ratio m_1/m_2 of the two species. Second, we report a novel segregation effect that occurs in the late stage of cooling, where interconnected domains appear. Spectral analysis of the composition field reveals…
The short-range correlations are considered for a two-dimensional hard-core boson model on square lattice within Bethe approximation for the clusters consisting of two and four sites. Explicit equations are derived for the critical temperatures of charge and superfluid ordering and their solutions are considered for various ratios of the charge-charge correlation parameter to the transfer integral. It is shown that taking into account short-range correlations for the temperatures of charge ordering results in the appearance of the critical concentration of bosons, which restricts the existence…
The analytical canonical NLT partition function of a quasi-one dimensional (q1D) system of hard disks [J. Chem Phys. v.153, 144111 (2020)] provides a direct analytical description of the thermodynamics and ordering in this system (a pore) as a function of the linear density N/L both for finite and infinite systems. It is alternative to the well-developed transfer matrix method based on the isobaric NPT ensemble. We derive the analytical formulae for the actual distance dependence of the translational pair distribution function (PDF) and the DF of distances between next neighbor disks, and then…
We study the dynamics of a system of hard-core particles sliding downwards on a one dimensional fluctuating interface, which in a special case can be mapped to the problem of a passive scalar advected by a Burgers fluid. Driven by the surface fluctuations, the particles show a tendency to cluster, but the hard-core interaction prevents collapse. We use numerical simulations to measure the auto-correlation function in steady state and in the aging regime, and space-time correlation functions in steady state. We have also calculated these quantities analytically in a related surface model. The s…
We argue that a system of straight rigid rods of length k on square lattice with only hard-core interactions shows two phase transitions as a function of density, rho, for k >= 7. The system undergoes a phase transition from the low-density disordered phase to a nematic phase as rho is increased from 0, at rho = rho_c1, and then again undergoes a reentrant phase transition from the nematic phase to a disordered phase at rho = rho_c2 < 1.
The new method of the mean-field approximation is extended. An approach which enables to estimate some parameters of the transition from the isotropic state of hard sticks to the nematic ordering phase is suggested. An technique of the investigation of the model jointed to the so-called polymer excluded volume problem is proposed. The critical exponents are estimated. The transition of a swelling polymer coil to ideal is revealed as the polymerization degree of the chain increases. The entanglement concentration obtained is in accordance with experimental data for polymers with flexible chains…
We show that one-dimensional topological objects (kinks) are natural degrees of freedom for an antiferromagnetic Ising model on a triangular lattice. Its ground states and the coexistence of spin ordering with an extensive zero-temperature entropy can be easily understood in terms of kinks forming a hard-sphere liquid. Using this picture we explain effects of quantum spin dynamics on that frustrated model, which we also study numerically.
