Density Distribution in Soft Matter Crystals and Quasicrystals.

The density distribution in solids is often represented as a sum of Gaussian peaks (or similar functions) centered on lattice sites or via a Fourier sum. Here, we argue that representing instead the logarithm of the density distribution via a Fourier sum is better. We show that truncating such a representation after only a few terms can be highly accurate for soft matter crystals. For quasicrystals, this sum does not truncate so easily, nonetheless, representing the density profile in this way is still of great use, enabling us to calculate the phase diagram for a three-dimensional quasicrystal-forming system using an accurate nonlocal density functional theory.

Which Wave Numbers Determine the Thermodynamic Stability of Soft Matter Quasicrystals?

For soft matter to form quasicrystals an important ingredient is to have two characteristic length scales in the interparticle interactions. To be more precise, for stable quasicrystals, periodic modulations of the local density distribution with two particular wave numbers should be favored, and the ratio of these wave numbers should be close to certain special values. So, for simple models, the answer to the title question is that only these two ingredients are needed. However, for more realistic models, where in principle all wave numbers can be involved, other wave numbers are also important, specifically those of the second and higher reciprocal lattice vectors. We identify features in the particle pair interaction potentials that can suppress or encourage density modes with wave numbers associated with one of the regular crystalline orderings that compete with quasicrystals, enabling either the enhancement or suppression of quasicrystals in a generic class of systems.

Three-Dimensional Icosahedral Phase Field Quasicrystal.

We investigate the formation and stability of icosahedral quasicrystalline structures using a dynamic phase field crystal model. Nonlinear interactions between density waves at two length scales stabilize three-dimensional quasicrystals. We determine the phase diagram and parameter values required for the quasicrystal to be the global minimum free energy state. We demonstrate that traits that promote the formation of two-dimensional quasicrystals are extant in three dimensions, and highlight the characteristics required for three-dimensional soft matter quasicrystal formation.

Soft-core particles freezing to form a quasicrystal and a crystal-liquid phase.

Systems of soft-core particles interacting via a two-scale potential are studied. The potential is responsible for peaks in the structure factor of the liquid state at two different but comparable length scales and a similar bimodal structure is evident in the dispersion relation. Dynamical density functional theory in two dimensions is used to identify two unusual states of this system: a crystal-liquid state, in which the majority of the particles are located on lattice sites but a minority remains free and so behaves like a liquid, and a 12-fold quasicrystalline state. Both are present even for deeply quenched liquids and are found in a regime in which the liquid is unstable with respect to modulations on the smaller scale only. As a result, the system initially evolves towards a small-scale crystal state; this state is not a minimum of the free energy, however, and so the system subsequently attempts to reorganize to generate the lower-energy larger-scale crystals. This dynamical process generates a disordered state with quasicrystalline domains and takes place even when this large scale is linearly stable, i.e., it is a nonlinear process. With controlled initial conditions, a perfect quasicrystal can form. The results are corroborated using Brownian dynamics simulations.

Quasicrystalline order and a crystal-liquid state in a soft-core fluid.

A two-dimensional system of soft particles interacting via a two-length-scale potential is studied. Density functional theory and Brownian dynamics simulations reveal a fluid phase and two crystalline phases with different lattice spacing. Of these the larger lattice spacing phase can form an exotic periodic state with a fraction of highly mobile particles: a crystal liquid. Near the transition between this phase and the smaller lattice spacing phase, quasicrystalline structures may be created by a competition between linear instability at one scale and nonlinear selection of the other.

Three-wave interactions and spatiotemporal chaos.

Three-wave interactions form the basis of our understanding of many pattern-forming systems because they encapsulate the most basic nonlinear interactions. In problems with two comparable length scales, it is possible for two waves of the shorter wavelength to interact with one wave of the longer, as well as for two waves of the longer wavelength to interact with one wave of the shorter. Consideration of both types of three-wave interactions can generically explain the presence of complex patterns and spatiotemporal chaos. Two length scales arise naturally in the Faraday wave experiment, and our results enable some previously unexplained experimental observations of spatiotemporal chaos to be interpreted in a new light. Our predictions are illustrated with numerical simulations of a model partial differential equation.

Skew-varicose instability in two-dimensional generalized Swift-Hohenberg equations.

We apply analytical and numerical methods to study the linear stability of stripe patterns in two generalizations of the two-dimensional Swift-Hohenberg equation that include coupling to a mean flow. A projection operator is included in our models to allow exact stripe solutions. In the generalized models, stripes become unstable to the skew-varicose, oscillatory skew-varicose, and cross-roll instabilities, in addition to the usual Eckhaus and zigzag instabilities. We analytically derive stability boundaries for the skew-varicose instability in various cases, including several asymptotic limits. We also use numerical techniques to determine eigenvalues and hence stability boundaries of other instabilities. We extend our analysis to both stress-free and no-slip boundary conditions and we note a crossover from the behavior characteristic of no-slip to that of stress-free boundaries as the coupling to the mean flow increases or as the Prandtl number decreases. Close to the critical value of the bifurcation parameter, the skew-varicose instability has the same curvature as the Eckhaus instability provided the coupling to the mean flow is greater than a critical value. The region of stable stripes is completely eliminated by the cross-roll instability for large coupling to the mean flow.

Quasipatterns in parametrically forced systems.

We examine two mechanisms that have been put forward to explain the selection of quasipatterns in single- and multifrequency forced Faraday wave experiments. Both mechanisms can be used to generate stable quasipatterns in a parametrically forced partial differential equation that shares some characteristics of the Faraday wave experiment. One mechanism, which is robust and works with single-frequency forcing, does not select a specific quasipattern: we find, for two different forcing strengths, 12-fold and 14-fold quasipatterns. The second mechanism, which requires more delicate tuning, can be used to select particular angles between wavevectors in the quasipattern.

Pattern formation in large domains.

Pattern formation is a phenomenon that arises in a wide variety of physical, chemical and biological situations. A great deal of theoretical progress has been made in understanding the universal aspects of pattern formation in terms of amplitudes of the modes that make up the pattern. Much of the theory has sound mathematical justification, but experiments and numerical simulations over the last decade have revealed complex two-dimensional patterns that do not have a satisfactory theoretical explanation. This paper focuses on quasi-patterns, where the appearance of small divisors causes the standard theoretical method to fail, and ends with a discussion of other outstanding problems in the theory of two-dimensional pattern formation in large domains.