arXiv subjects

M. Widom

Publications and source records attributed to M. Widom.

At least 37 records · Page 2Linked to original sources

arXiv2006

Signature of nearly icosahedral structures in liquid and supercooled liquid Copper

A growing body of experiments display indirect evidence of icosahedral structures in supercooled liquid metals. Computer simulations provide more direct evidence but generally rely on approximate interatomic potentials of unproven accuracy. We use first-principles molecular dynamics simulations to generate realistic atomic configurations, providing structural detail not directly available from experiment, based on interatomic forces that are more reliable than conventional simulations. We analyze liquid copper, for which recent experimental results are available for comparison, to quantify the degree of local icosahedral and polytetrahedral order.

cond-mat.mtrl-sci↗

arXiv2005

Random tilings of high symmetry: I. Mean-field theory

We study random tiling models in the limit of high rotational symmetry. In this limit a mean-field theory yields reasonable predictions for the configurational entropy of free boundary rhombus tilings in two dimensions. We base our mean-field theory on an iterative tiling construction inspired by the work of de Bruijn. In addition to the entropy, we consider correlation functions, phason elasticity and the thermodynamic limit. Tilings of dimension other than two are considered briefly.

cond-mat.stat-mech↗

arXiv2004

Stability of Fe-based alloys with structure type C6Cr23

Bulk metallic glass forms when liquid metal alloys solidify without crystalization. In the search for Iron-based bulk glass-forming alloys of the metal-metalloid type (Fe-B- and Fe-C-based), crystals based on the structural prototype C6Cr23 often preempt the amorphous phase. Destabilizing this competing crystal structure could enhance glass-formability. We carry out first-principles total energy calculations of enthalpy of formation to identify third elements that can effectively destabilize C6Cr23. Yttrium appears optimal among transition metals, and rare earths also are suitable. Atomic size is the dominant factor.

cond-mat.mtrl-sci↗

arXiv2004

First-principles prediction of a decagonal quasicrystal containing boron

We interpret experimentally known B-Mg-Ru crystals as quasicrystal approximants. These approximant structures imply a deterministic decoration of tiles by atoms that can be extended quasiperiodically. Experimentally observed structural disorder corresponds to phason (tile flip) fluctuations. First-principles total energy calculations reveal that many distinct tilings lie close to stability at low temperatures. Transfer matrix calculations based on these energies suggest a phase transition from a crystalline state at low temperatures to a high temperature state characterized by tile fluctuations. We predict B$_{38}$Mg$_{17}$Ru$_{45}$ forms a decagonal quasicrystal that is metastable at low temperatures and may be thermodynamically stable at high temperatures.

cond-mat.mtrl-sci↗

arXiv2004

Cohesive energies of Fe-based glass-forming alloys

We calculate the cohesive energies of Fe-based glass-forming alloys in the B-Fe-Y-Zr quaternary system. Our {\it ab-initio} calculations fully relax atomic positions and lattice parameters yielding enthalpies of mixing at T=0K. We examine both the known equilibrium and metastable phases as well as a selection of plausible structures drawn from related alloy systems. This method, generally reproduces experimentally determined phase diagrams while providing additional information about energetics of metastable and unstable structures. In particular we can identify crystalline structures whose formation competes with the metallic glass. In some cases we identify previously unknown structures or observe possible errors in the experimental phase diagrams.

cond-mat.mtrl-sci↗

arXiv2004

Equilibrium structure of decagonal AlNiCo

We investigate the high temperature decagonal quasicrystalline phase of Al$_{72}$Ni$_{20}$Co$_8$ using a quasilattice gas Monte-Carlo simulation. To avoid biasing towards a specific model we use an over-dense site list with a large fraction of free sites, permitting the simulation to explore an extended region of perpendicular space. Representing the atomic surface occupancy in a basis of harmonic functions directly reveals the 5-fold symmetric component of our data. Occupancy is examined in physical and perpendicular space.

cond-mat.mtrl-sci↗

arXiv2004

Order-disorder transition in the Cd-Ca cubic approximant

Recent experiments discovered an order-disorder transition occuring at low temperatures in large unit 1/1 cell cubic approximants of the stable Cd-based binary alloy quasicrystals. The transition is related to correlations among orientational degrees of freedom whose separations are around 12 Å. We analyze the interactions between the degrees of freedom using {\em ab-initio} calculations for Cd-Ca alloys and derive an equivalent antiferromagnetic Ising model which shows a similar phase transition. However, the calculated transition temperature is higher than observed experimentally, indicating that the actual structure and its order-disorder transition are more complex than originally proposed. A side-benefit of our study is the discovery of a canonical-cell decoration model for the Cd-Ca icosahedral phase.

cond-mat.mtrl-sci↗

arXiv2004

Quasicrystal approximants with novel compositions and structures

We identify several new quasicrystal approximants in alloy systems in which quasicrystals have not been previously reported. Some occur in alloys with large size contrast between the constituent elements, either containing small Boron atoms, or large Ca/Eu atoms, leading to quasicrystal structures quite different from currently known systems where the size contrast is smaller. Another group of the approximants are layered Frank--Kasper structures, demonstrating competition between decagonal and dodecagonal ordering within this family of structures.

cond-mat.mtrl-sci↗

arXiv2003

Combined energy -- diffraction data refinement of decagonal AlNiCo

We incorporate realistic pair potential energies directly into a non-linear least-square fit of diffraction data to quantitatively compare structure models with experiment for the Ni-rich $d$(AlNiCo) quasicrystal. The initial structure models are derived from a few {\it a priori} assumptions (gross features of the Patterson function) and the pair potentials. In place of the common hyperspace approach to the structure refinement of quasicrystals, we use a real-space tile decoration scheme, which does not rely on strict quasiperiodicity, and makes it easy to enforce sensible local arrangements of the atoms. Inclusion of the energies provides information complementary to the diffraction data and protects the fit procedure from converging on spurious solutions. The method pinpoints sites which are likely to break the symmetry of their local environment.

cond-mat.mtrl-sci↗

arXiv2003

Arctic octahedron in three-dimensional rhombus tilings and related integer solid partitions

Three-dimensional integer partitions provide a convenient representation of codimension-one three-dimensional random rhombus tilings. Calculating the entropy for such a model is a notoriously difficult problem. We apply transition matrix Monte Carlo simulations to evaluate their entropy with high precision. We consider both free- and fixed-boundary tilings. Our results suggest that the ratio of free- and fixed-boundary entropies is $σ_{free}/σ_{fixed}=3/2$, and can be interpreted as the ratio of the volumes of two simple, nested, polyhedra. This finding supports a conjecture by Linde, Moore and Nordahl concerning the ``arctic octahedron phenomenon'' in three-dimensional random tilings.

cond-mat.stat-mech↗

arXiv2002

Tile Hamiltonians for Decagonal Phases

A tile Hamiltonian (TH) replaces the actual atomic interactions in a quasicrystal with effective interactions between and within tiles. We study Al-Co-Ni and Al-Co-Cu decagonal quasicrystals described as decorated Hexagon-Boat-Star (HBS) tiles using {\em ab-initio} methods. A dominant term in the TH counts the number of H, B and S tiles, favoring tilings of H and B only. In our model for Al-Co-Cu, chemical ordering of Cu and Co along tile edges defines tile edge arrowing. Unlike the edge arrowing of Penrose matching rules, however, the energetics for Al-Co-Cu do not force quasiperiodicity. Energetically favored structures resemble crystalline approximants to which the actual quasicrystalline compounds transform at low temperature.

cond-mat↗

arXiv2001

Shapes and textures of ferromagnetic liquid droplets

Theoretical calculations, computer simulations and experiments indicate the possible existence of a ferromagnetic liquid state. Should such a state exist, demagnetization effects would force a nontrivial magnetization texture governed by the shape of the liquid droplet. Since liquid droplets are deformable, the droplet shape couples to the magnetization texture. This paper solves the joint shape/texture problem subject to the assumption of cylindrical droplet symmetry. The shape undergoes a change in topology from spherical to toroidal as exchange energy grows or surface tension decreases.

cond-mat.soft↗

arXiv2001

Total-energy-based prediction of a quasicrystal structure

Quasicrystals are metal alloys whose noncrystallographic symmetry and lack of structural periodicity challenge methods of experimental structure determination. Here we employ quantum-based total-energy calculations to predict the structure of a decagonal quasicrystal from first principles considerations. We employ Monte Carlo simulations, taking as input the knowledge that a decagonal phase occurs in Al-Ni-Co near a given composition, and using a few features of the experimental Patterson function. The resulting structure obeys a nearly deterministic decoration of tiles on a hierarchy of length scales related by powers of $τ$, the golden mean.

cond-mat↗

arXiv2000

Thermodynamic Limit for Polydisperse Fluids

We examine the thermodynamic limit of fluids of hard core particles that are polydisperse in size and shape. In addition, particles may interact magnetically. Free energy of such systems is a random variable because it depends on the choice of particles. We prove that the thermodynamic limit exists with probability 1, and is independent of the choice of particles. Our proof applies to polydisperse hard-sphere fluids, colloids and ferrofluids. The existence of a thermodynamic limit implies system shape and size independence of thermodynamic properties of a system.

cond-mat.stat-mech↗

arXiv2000

Thermodynamic Limit for Dipolar Media

We prove existence of a shape and boundary condition independent thermodynamic limit for fluids and solids of identical particles with electric or magnetic dipole moments. Our result applies to fluids of hard core particles, to dipolar soft spheres and Stockmayer fluids, to disordered solid composites, and to regular crystal lattices. In addition to their permanent dipole moments, particles may further polarize each other. Classical and quantum models are treated. Shape independence depends on the reduction in free energy accomplished by domain formation, so our proof applies only in the case of zero applied field. Existence of a thermodynamic limit implies texture formation in spontaneously magnetized liquids and disordered solids analogous to domain formation in crystalline solids.

cond-mat.stat-mech↗

arXiv1999

Two-dimensional random tilings of large codimension: new progress

Two-dimensional random tilings of rhombi can be seen as projections of two-dimensional membranes embedded in hypercubic lattices of higher dimensional spaces. Here, we consider tilings projected from a $D$-dimensional space. We study the limiting case, when the quantity $D$, and therefore the number of different species of tiles, become large. We had previously demonstrated [ICQ6] that, in this limit, the thermodynamic properties of the tiling become independent of the boundary conditions. The exact value of the limiting entropy and finite $D$ corrections remain open questions. Here, we develop a mean-field theory, which uses an iterative description of the tilings based on an analogy with avoiding oriented walks on a random tiling. We compare the quantities so-obtained with numerical calculations. We also discuss the role of spatial correlations.

cond-mat.stat-mech↗

arXiv1999

Ferromagnetic Liquid Thin Films Under Applied Field

Theoretical calculations, computer simulations and experiments indicate the possible existence of a ferromagnetic liquid state, although definitive experimental evidence is lacking. Should such a state exist, demagnetization effects would force a nontrivial magnetization texture. Since liquid droplets are deformable, the droplet shape is coupled with the magnetization texture. In a thin-film geometry in zero applied field, the droplet has a circular shape and a rotating magnetization texture with a point vortex at the center. We calculate the elongation and magnetization texture of such ferromagnetic thin film liquid droplet confined between two parallel plates under a weak applied magnetic field. The vortex stretches into a domain wall and exchange forces break the reflection symmetry. This behavior contrasts qualitatively and quantitatively with the elongation of paramagnetic thin films.

cond-mat.soft↗

arXiv1999

Parallel flow in Hele-Shaw cells with ferrofluids

Parallel flow in a Hele-Shaw cell occurs when two immiscible liquids flow with relative velocity parallel to the interface between them. The interface is unstable due to a Kelvin-Helmholtz type of instability in which fluid flow couples with inertial effects to cause an initial small perturbation to grow. Large amplitude disturbances form stable solitons. We consider the effects of applied magnetic fields when one of the two fluids is a ferrofluid. The dispersion relation governing mode growth is modified so that the magnetic field can destabilize the interface even in the absence of inertial effects. However, the magnetic field does not affect the speed of wave propagation for a given wavenumber. We note that the magnetic field creates an effective interaction between the solitons.

cond-mat.soft↗