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

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