Jamming Research Papers - Academia.edu (original) (raw)
In quenched disordered out-of-equilibrium many-body colloidal systems, there are important distinctions between the glass transition, which is related to the onset of nonergodicity and loss of low-frequency relaxations caused by crowding,... more
In quenched disordered out-of-equilibrium many-body colloidal systems, there are important distinctions between the glass transition, which is related to the onset of nonergodicity and loss of low-frequency relaxations caused by crowding, and the jamming transition, which is related to the dramatic increase in elasticity of the system caused by the deformation of constituent objects. For softer repulsive interaction potentials, these two transitions become increasingly smeared together, so measuring a clear distinction between where the glass ends and where jamming begins becomes very difficult or even impossible. Here, we investigate droplet dynamics in concentrated silicone oil-in-water nanoemulsions using light scattering. For zero or low NaCl electrolyte concentrations, interfacial repulsions are soft and longer in range, this transition sets in at lower concentrations, and the glass and the jamming regimes are smeared. However, at higher electrolyte concentrations the interactions are stiffer, and the characteristics of the glass-jamming transition resemble more closely the situation of disordered elastic spheres having sharp interfaces, so the glass and jamming regimes can be distinguished more clearly. The glass and jamming transitions of colloidal repulsive hard and soft spheres have been the subject of numerous studies over the last decades. These studies have been conducted in order to address fundamental questions related to the microscopic mechanisms of crystallization and glass formation in condensed matter physics 1–8. The crystalline phase has the lowest free energy and is in thermodynamic equilibrium, but a long-lived amorphous glassy state is readily obtained whenever crystallization is frustrated by a nonuniform particle size distribution or by a rapid quench to raise the volume fraction of the dispersed particles, φ. In the case of a rapid quench of mon-odisperse hard spheres, the standard scenario suggests that for a volume fraction of spheres associated with a glass transition, 0 58 g φ. , a weak glassy state is formed, the viscosity diverges η → ∞, and a finite low-frequency elastic shear modulus develops, ∼ G k T R / B 0 3 , for spheres having an average radius R. Further increasing the density , the particles can touch and jam, forming a space filling network of contact forces 9. Contact forces are typical of granular materials composed of non-colloidal grains, but are not strictly valid for stable dispersions of colloidal particles in a viscous liquid. In such colloidal dispersions, the particles diffuse under the influence of thermal fluctuations and are stabilized against irreversible aggregation by short-range slippery repulsive interactions that preclude strict solid-solid frictional contact in quiescent conditions. Often, thermal or Brownian fluctuations are justifiably neglected in non-colloidal granular systems, yet these fluctuations are a measure for the influence of entropy and can be important in colloidal soft matter composed of dispersed spherical objects, including dispersions of hard nanospheres as well as nanoemulsions of deformable droplets of one liquid (e.g. oil) dispersed in an immiscible liquid (e.g. water) stabilized against coalescence by adsorbed surfactant molecules. The glass transition can be understood by the formation and fluctuation of long-lived cages of particles over many length scales; a disordered system of monodisperse spheres can be formed by raising φ rapidly enough above a value φ g to preclude the colloidal disorder-order transition known for hard spheres 10,11 , and the disordered glassy system self-adjusts given the available space and maximizes entropy subject to non-equilibrium constraints which can preclude crystal formation. By contrast, jamming is associated with direct repulsive Published: xx xx xxxx OPEN