We report Monte Carlo simulations of phase behavior of colloidal suspensions with near-critical binary solvents using effective pair potentials from experiments. At off-critical solvent composition, the calculated phase diagram agrees well with measurements of the experimental system, indicating that many-body effects are limited. Close to the critical composition, however, agreement between experiment and simulation becomes poorer, signaling the increased importance of many-body effects. Both at and off the critical solvent concentration, the colloidal phase diagram is qualitatively similar to those of molecular systems and obeys the principle of corresponding states with one striking difference: it occurs in a narrow temperature interval of <1 • C below the solvent phase separation temperature.

Glasses acquire their solid-like properties by cooling from the supercooled liquid via a continuous transition known as the glass transition. Recent research on soft glasses indicates that besides temperature, another route to liquify glasses is by application of stress that drives relaxation and flow. Here, we show that unlike the continuous glass transition, the failure of glasses to applied stress occurs by a sharp symmetry change that reminds of first-order equilibrium transitions. Using simultaneous x-ray scattering during the oscillatory rheology of a colloidal glass, we identify a sharp symmetry change from anisotropic solid to isotropic liquid structure at the crossing of the storage and loss moduli. Concomitantly, intensity fluctuations sharply acquire Gaussian distributions characteristic of liquids. Our observations and theoretical framework identify mechanical failure as a sharp atomic affine-to-nonaffine transition, providing a new conceptual paradigm of the oscillatory yielding of this technologically important class of materials, and offering new perspectives on the glass transition.

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General rightsIt is not permitted to download or to forward/distribute the text or part of it without the consent of the author(s) and/or copyright holder(s), other than for strictly personal, individual use, unless the work is under an open content license (like Creative Commons). Disclaimer/Complaints regulationsIf you believe that digital publication of certain material infringes any of your rights or (privacy) interests, please let the Library know, stating your reasons. In case of a legitimate complaint, the Library will make the material inaccessible and/or remove it from the website. Please Ask the Library: http://uba.uva.nl/en/contact, or a letter to: Library of the University of Amsterdam, Secretariat, Singel 425, 1012 WP Amsterdam, The Netherlands. You will be contacted as soon as possible. We employ x-ray scattering on sheared colloidal suspensions and mode coupling theory to study structure factor distortions of glass-forming systems under shear. We find a transition from quadrupolar elastic distortion at small strains to quadrupolar and hexadecupolar modes in the stationary state. The latter are interpreted as signatures of plastic rearrangements in homogeneous, thermalized systems. From their transient evolution with strain, we identify characteristic strain and length-scale values where these plastic rearrangements dominate. This characteristic strain coincides with the maximum of the shear stress versus strain curve, indicating the proliferation of plastic flow. The hexadecupolar modes dominate at the wavevector of the principal peak of the equilibrium structure factor that is related to the cage-effect in mode coupling theory. We hence identify the structural signature of plastic flow of glasses. C 2015 AIP Publishing LLC.[http://dx

Glasses have liquid-like structure, but exhibit solid-like properties. A central question concerns the relation between the structure and mechanical properties of glasses, but structural changes remain difficult to resolve. We use a novel combination of rheology and x-ray scattering to resolve structural changes in colloidal glasses and link them directly to their mechanical behavior. By combining stress and structure factor measurements, we resolve shear induced changes in the nearest neighbor configuration as a function of applied stress, allowing us to elucidate the structural origin of the genuine shear banding transition of glasses.