Crystalline Phases of Polydisperse Spheres

We use specialized Monte Carlo simulation methods and moment free energy calculations to provide conclusive evidence that dense polydisperse spheres at equilibrium demix into coexisting fcc phases, with more phases appearing as the spread of diameters increases. We manage to track up to four coexisting phases. Each of these is fractionated: it contains a narrower distribution of particle sizes than is present in the system overall. We also demonstrate that, surprisingly, demixing transitions can be nearly continuous, accompanied by fluctuations in local particle size correlated over many lattice spacings.