Crystallization of hard-sphere colloids: deviations from classical nucleation theory

The creation of three-dimensional ordered colloidal crystals, for application in a range of nanotechnologies, has been a goal for many researchers in the past few years. The main difficulty in creating macroscopic sized crystals of densely packed colloidal particles is that colloidal particles always have a range of particle sizes - ie, they are polydisperse. This paper studied the crystallization kinetics of a hard-sphere colloid with a well defined Gaussian polydispersity. The authors find that crystallization occurs in two stages, and does not follow the simple classical nucleation picture. The paper discusses the implications of these results for research into colloidal crystals as possible nano-materials

Small changes in particle-size distribution dramatically delay and enhance nucleation in hard sphere colloidal suspensions

We present hard-sphere crystallization kinetics for three samples with small differences in polydispersity. We show that an increase in polydispersity of 1% is sufficient to cause dramatic changes in the crystallization kinetics: Crystallization is delayed by almost one decade in time and quantitative and qualitative changes in the crystallization scenario are observed. Surprisingly the nucleation rate density is enhanced by almost a factor of 10. We interpret these results in terms of polydispersity limited growth, where local fractionation processes lead to a delayed but faster nucleation

Effect of polydispersity on the crystallization kinetics of suspensions of colloidal hard spheres when approaching the glass transition

We present a comprehensive study of the solidification scenario in suspensions of colloidal hard spheres for three polydispersities between 4.8% and 5.8%, over a range of volume fractions from near freezing to near the glass transition. From these results, we identify four stages in the crystallization process: (i) an induction stage where large numbers of precursor structures are observed, (ii) a conversion stage as precursors are converted to close packed structures, (iii) a nucleation stage, and (iv) a ripening stage. It is found that the behavior is qualitatively different for volume fractions below or above the melting volume fraction. The main effect of increasing polydispersity is to increase the duration of the induction stage, due to the requirement for local fractionation of particles of larger or smaller than average size. Near the glass transition, the nucleation process is entirely frustrated, and the sample is locked into a compressed crystal precursor structure. Interestingly, neither polydispersity nor volume fraction significantly influences the precursor stage, suggesting that the crystal precursors are present in all solidifying samples. We speculate that these precursors are related to the dynamical heterogeneities observed in a number of dynamical studies

Preparation and characterization of particles with small differences in polydispersity

Colloidal particles are widely used both in fundamental research and in materials science. One important parameter influencing the physical properties of colloidal materials is the particle size distribution (polydispersity) of the colloidal particles. Recent work on colloidal crystallization has demonstrated that even subtle changes in polydispersity can have significant effects. In this study we present centrifugation techniques for subtly manipulating the width and the shape of the particle size distribution, for polydispersities less than 10%. We use scanning electron microscopy as well as dynamic and static light scattering to characterize the particle size distributions. We compare the results and highlight the difficulties associated with the determination of accurate particle size distributions

Coulomb gap in a model with finite charge transfer energy

The Coulomb gap in a donor-acceptor model with finite charge transfer energy $\Delta$ describing the electronic system on the dielectric side of the metal-insulator transition is investigated by means of computer simulations on two- and three-dimensional finite samples with a random distribution of equal amounts of donor and acceptor sites. Rigorous relations reflecting the symmetry of the model presented with respect to the exchange of donors and acceptors are derived. In the immediate neighborhood of the Fermi energy $\mu$ the the density of one-electron excitations $g(\epsilon)$ is determined solely by finite size effects and $g(\epsilon)$ further away from $\mu$ is described by an asymmetric power law with a non-universal exponent, depending on the parameter $\Delta$.Comment: 10 pages, 6 figures, submitted to Phys. Rev.

Propagation of first sound in liquid 3He

The dispersion of first (hydrodynamic) sound in normalfluid and superfluid 3He has been measured in a cylindrical resonator at a pressure of 18.8 bar in the frequency range between 85 kHz and 227 kHz and in the temperature range between 1.2 and 50 mK. The sound velocity measured in the normalfluid regime confirms recent theories of the slip effect in Fermi liquids; in superfluid 3He-B we find qualitative agreement between experiment and theoretical sound velocity

Evidence for a superfluid-induced surface barrier for electrons in liquid helium

The free surface of liquid helium acts as an energy barrier on electron currents across the surface into the vapor, if the liquid is superfluid. In zero electric field, the barrier vanishes at Tλ. The measurements were performed in pure 4He in 4He