Quasicrystal of Binary Hard Spheres on a Plane Stabilized by Configurational Entropy

Because of their aperiodic nature, quasicrystals are one of the least understood phases in statistical physics. One significant complication they present in comparison to their periodic counterparts is the fact that any quasicrystal can be realized as an exponentially large number of different tilings, resulting in a significant contribution to the quasicrystal entropy. Here, we use free-energy calculations to demonstrate that it is this configurational entropy which stabilizes a dodecagonal quasicrystal in a binary mixture of hard spheres on a plane. Our calculations also allow us to quantitatively confirm that in this system all tiling realizations are essentially equally likely, with free-energy differences less than 0.0001kBT per particle—an observation that could be related to the observation of only random tilings in soft-matter quasicrystals. Owing to the simplicity of the model and its available counterparts in colloidal experiments, we believe that this system is an excellent candidate to achieve the long-awaited quasicrystal self-assembly on the micron scale.Received 6 June 2023Revised 8 September 2023Accepted 3 January 2024DOI:https://doi.org/10.1103/PhysRevLett.132.048202© 2024 American Physical SocietyPhysics Subject Headings (PhySH)Research AreasPhase behaviorPhysical SystemsColloidal crystalHard sphere colloidsPolymers & Soft Matter