Self-assembly of dodecagonal and octagonal quasicrystals in hard spheres on a plane

Hard spheres are one of the most fundamental model systems in soft matter physics, and have been instrumental in shedding light on nearly every aspect of classical condensed matter. Here, we add one more important phase to the list that hard spheres form: quasicrystals. Specifically, we use simulations to show that an extremely simple, purely entropic model system, consisting of two sizes of hard spheres resting on a flat plane, can spontaneously self-assemble into two distinct random-tiling quasicrystal phases. The first quasicrystal is a dodecagonal square-triangle tiling, commonly observed in a large variety of colloidal systems. The second quasicrystal has, to our knowledge, never been observed in either experiments or simulations. It exhibits octagonal symmetry, and consists of three types of tiles: triangles, small squares, and large squares, whose relative concentration can be continuously varied by tuning the number of smaller spheres present in the system. The observed tile composition of the self-assembled quasicrystals agrees very well with the theoretical prediction we obtain by considering the four-dimensional (lifted) representation of the quasicrystal. Both quasicrystal phases form reliably and rapidly over a significant part of parameter space. Our results demonstrate that entropy combined with a set of geometrically compatible, densely packed tiles can be sufficient ingredients for the self-assembly of colloidal quasicrystals.