Stability of Soft Quasicrystals in a Coupled-Mode Swift-Hohenberg Model for Three-Component Systems

In this article, we discuss the stability of soft quasicrystalline phases in a coupled-mode Swift-Hohenberg model for three-component systems, where the characteristic length scales are governed by the positive-definite gradient terms. Classic two-mode approximation method and direct numerical minimization are applied to the model. In the latter approach, we apply the projection method to deal with the potentially quasiperiodic ground states. A variable cell method of optimizing the shape and size of higher-dimensional periodic cell is developed to minimize the free energy with respect to the order parameters. Based on the developed numerical methods, we rediscover decagonal and dodecagonal quasicrystalline phases, and find diverse periodic phases and complex modulated phases. Furthermore, phase diagrams are obtained in various phase spaces by comparing the free energies of different candidate structures. It does show not only the important roles of system parameters, but also the effect of optimizing computational domain. In particular, the optimization of computational cell allows us to capture the ground states and phase behavior with higher fidelity. We also make some discussions on our results and show the potential of applying our numerical methods to a larger class of mean-field free energy functionals.Comment: 26 pages, 13 figures; accepted by Communications in Computational Physic

Stability of Two-Dimensional Soft Quasicrystals

The relative stability of two-dimensional soft quasicrystals is examined using a recently developed projection method which provides a unified numerical framework to compute the free energy of periodic crystal and quasicrystals. Accurate free energies of numerous ordered phases, including dodecagonal, decagonal and octagonal quasicrystals, are obtained for a simple model, i.e. the Lifshitz-Petrich free energy functional, of soft quasicrystals with two length-scales. The availability of the free energy allows us to construct phase diagrams of the system, demonstrating that, for the Lifshitz-Petrich model, the dodecagonal and decagonal quasicrystals can become stable phases, whereas the octagonal quasicrystal stays as a metastable phase.Comment: 11 pages, 7 figure

Multiple-scale structures: from Faraday waves to soft-matter quasicrystals

For many years, quasicrystals were observed only as solid-state metallic alloys, yet current research is now actively exploring their formation in a variety of soft materials, including systems of macromolecules, nanoparticles and colloids. Much effort is being invested in understanding the thermodynamic properties of these soft-matter quasicrystals in order to predict and possibly control the structures that form, and hopefully to shed light on the broader yet unresolved general questions of quasicrystal formation and stability. Moreover, the ability to control the self-assembly of soft quasicrystals may contribute to the development of novel photonic or other applications based on self-assembled metamaterials. Here a path is followed, leading to quantitative stability predictions, that starts with a model developed two decades ago to treat the formation of multiple-scale quasiperiodic Faraday waves (standing wave patterns in vibrated fluid surfaces) and which was later mapped onto systems of soft particles, interacting via multiple-scale pair potentials. The article reviews, and substantially expands, the quantitative predictions of these models, while correcting a few discrepancies in earlier calculations, and presents new analytical methods for treating the models. In so doing, a number of new stable quasicrystalline structures with octagonal, octadecagonal and higher-order symmetries, some of which may, it is hoped, be observed in future experiments.Comment: 22 pages, 22 figures, 1 table. Comments welcom

Stability of Quasicrystals Composed of Soft Isotropic Particles

Quasicrystals whose building blocks are of mesoscopic rather than atomic scale have recently been discovered in several soft-matter systems. Contrary to metallurgic quasicrystals whose source of stability remains a question of great debate to this day, we argue that the stability of certain soft-matter quasicrystals can be directly explained by examining a coarse-grained free energy for a system of soft isotropic particles. We show, both theoretically and numerically, that the stability can be attributed to the existence of two natural length scales in the pair potential, combined with effective three-body interactions arising from entropy. Our newly gained understanding of the stability of soft quasicrystals allows us to point at their region of stability in the phase diagram, and thereby may help control the self-assembly of quasicrystals and a variety of other desired structures in future experimental realizations.Comment: Revised abstract, more detailed explanations, and better images of the numerical minimization of the free energ

Self-assembly of two-dimensional binary quasicrystals: A possible route to a DNA quasicrystal

We use Monte Carlo simulations and free-energy techniques to show that binary solutions of penta- and hexavalent two-dimensional patchy particles can form thermodynamically stable quasicrystals even at very narrow patch widths, provided their patch interactions are chosen in an appropriate way. Such patchy particles can be thought of as a coarse-grained representation of DNA multi-arm `star' motifs, which can be chosen to bond with one another very specifically by tuning the DNA sequences of the protruding arms. We explore several possible design strategies and conclude that DNA star tiles that are designed to interact with one another in a specific but not overly constrained way could potentially be used to construct soft quasicrystals in experiment. We verify that such star tiles can form stable dodecagonal motifs using oxDNA, a realistic coarse-grained model of DNA

Numerical Methods for Quasicrystals

Quasicrystals are one kind of space-filling structures. The traditional crystalline approximant method utilizes periodic structures to approximate quasicrystals. The errors of this approach come from two parts: the numerical discretization, and the approximate error of Simultaneous Diophantine Approximation which also determines the size of the domain necessary for accurate solution. As the approximate error decreases, the computational complexity grows rapidly, and moreover, the approximate error always exits unless the computational region is the full space. In this work we focus on the development of numerical method to compute quasicrystals with high accuracy. With the help of higher-dimensional reciprocal space, a new projection method is developed to compute quasicrystals. The approach enables us to calculate quasicrystals rather than crystalline approximants. Compared with the crystalline approximant method, the projection method overcomes the restrictions of the Simultaneous Diophantine Approximation, and can also use periodic boundary conditions conveniently. Meanwhile, the proposed method efficiently reduces the computational complexity through implementing in a unit cell and using pseudospectral method. For illustrative purpose we work with the Lifshitz-Petrich model, though our present algorithm will apply to more general systems including quasicrystals. We find that the projection method can maintain the rotational symmetry accurately. More significantly, the algorithm can calculate the free energy density to high precision.Comment: 27 pages, 8 figures, 6 table

Universal self-assembly of one-component three-dimensional dodecagonal quasicrystals

Using molecular dynamics simulations, we study computational self-assembly of one-component three-dimensional dodecagonal (12-fold) quasicrystals in systems with two-length-scale potentials. Existing criteria for three-dimensional quasicrystal formation are quite complicated and rather inconvenient for particle simulations. So to localize numerically the quasicrystal phase, one should usually simulate over a wide range of system parameters. We show how to universally localize the parameters values at which dodecagonal quasicrystal order may appear for a given particle system. For that purpose, we use a criterion recently proposed for predicting decagonal quasicrystal formation in one-component two-length-scale systems. The criterion is based on two dimensionless effective parameters describing the fluid structure which are extracted from radial distribution function. The proposed method allows reducing the time spent for searching the parameters favoring certain solid structure for a given system. We show that the method works well for dodecagonal quasicrystals; this results is verified on four systems with different potentials: Dzugutov potential, oscillating potential which mimics metal interactions, repulsive shoulder potential describing effective interaction for core/shell model of colloids and embedded-atom model potential for aluminum. Our results suggest that mechanism of dodecagonal quasicrystal formation is universal for both metallic and soft-matter systems and it is based on competition between interparticle scales.Comment: 8 pages, 6 figure

Controlled self-assembly of periodic and aperiodic cluster crystals

Soft particles are known to overlap and form stable clusters that self-assemble into periodic crystalline phases with density-independent lattice constants. We use molecular dynamics simulations in two dimensions to demonstrate that, through a judicious design of an isotropic pair potential, one can control the ordering of the clusters and generate a variety of phases, including decagonal and dodecagonal quasicrystals. Our results confirm analytical predictions based on a mean-field approximation, providing insight into the stabilization of quasicrystals in soft macromolecular systems, and suggesting a practical approach for their controlled self-assembly in laboratory realizations using synthesized soft-matter particles.Comment: Supplemental Material can be obtained through the author's website at: http://www.tau.ac.il/~ronlif/pubs/ClusterCrystals-Supp.pd