Self-assembly of spiral patterns in confined systems with competing interactions

Colloidal particles in polymer solutions and functionalized nanoparticles often exhibit short-range attraction coupled with long-range repulsion (SALR) leading to the spontaneous formation of symmetric patterns. Chiral nanostructures formed by thin films of SALR particles have not been reported yet. In this study, we observe striking topological transitions from a symmetric pattern of concentric rings to a chiral structure of a spiral shape, when the system is in hexagonal confinement. We find that the spiral formation can be induced either by breaking the system symmetry with a wedge, or by melting of the rings. In the former case, the chirality of the spiral is determined by the orientation of the wedge and thus can be controlled. In the latter, the spiral arises due to thermally induced defects and is absent in the average particle distribution, which forms highly regular hexagonal patterns in the central part of the system. These hexagonal patterns can be explained by interference of planar density waves. Thermodynamic considerations indicate that equilibrium spirals can appear spontaneously in any stripe-forming system confined in a hexagon with a small wedge, provided that certain conditions are satisfied by a set of phenomenological parameters.