Using dynamical density functional theory we calculate the speed of solidification fronts advancing into a quenched two-dimensional model fluid of soft-core particles. We find that solidification fronts can advance via two different mechanisms, depending on the depth of the quench. For shallow quenches, the front propagation is via a nonlinear mechanism. For deep quenches, front propagation is governed by a linear mechanism and in this regime we are able to determine the front speed via a marginal stability analysis. We find that the density modulations generated behind the advancing front have a characteristic scale that differs from the wavelength of the density modulation in thermodynamic equilibrium, i.e., the spacing between the crystal planes in an equilibrium crystal. This leads to the subsequent development of disorder in the solids that are formed. For the onecomponent fluid, the particles are able to rearrange to form a well-ordered crystal, with few defects. However, solidification fronts in a binary mixture exhibiting crystalline phases with square and hexagonal ordering generate solids that are unable to rearrange after the passage of the solidification front and a significant amount of disorder remains in the system.
We investigate the liquid state structure of the two-dimensional model introduced by Barkan et al. [Phys. Rev. Lett. 113, 098304 (2014)10.1103/PhysRevLett.113.098304], which exhibits quasicrystalline and other unusual solid phases, focusing on the radial distribution function g(r) and its asymptotic decay r→∞. For this particular model system, we find that as the density is increased there is a structural crossover from damped oscillatory asymptotic decay with one wavelength to damped oscillatory asymptotic decay with another distinct wavelength. The ratio of these wavelengths is ≈1.932. Following the locus in the phase diagram of this structural crossover leads directly to the region where quasicrystals are found. We argue that identifying and following such a crossover line in the phase diagram towards higher densities where the solid phase(s) occur is a good strategy for finding quasicrystals in a wide variety of systems. We also show how the pole analysis of the asymptotic decay of equilibrium fluid correlations is intimately connected with the nonequilibrium growth or decay of small-amplitude density fluctuations in a bulk fluid.
We show how deeply quenching a liquid to temperatures where it is linearly unstable and the crystal is the equilibrium phase often produces crystalline structures with defects and disorder. As the solid phase advances into the liquid phase, the modulations in the density distribution created behind the advancing solidification front do not necessarily have a wavelength that is the same as the equilibrium crystal lattice spacing. This is because in a deep enough quench the front propagation is governed by linear processes, but the crystal lattice spacing is determined by nonlinear terms. The wavelength mismatch can result in significant disorder behind the front that may or may not persist in the latter stage dynamics. We support these observations by presenting results from dynamical density functional theory calculations for simple one-and two-component two-dimensional systems of soft core particles.
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