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David R. Reichman

Publications and source records attributed to David R. Reichman.

175 records · Page 10Linked to original sources

Short-ranged attractions in jammed liquids: How cooling can melt a glass

We demonstrate that an extended picture of kinetic constraints in glass-forming liquids is sufficient to explain dynamic anomalies observed in dense suspensions of strongly attracting colloidal particles. We augment a simple model of heterogeneous relaxation with static attractions between facilitating excitations, in a way that mimics the structural effect of short-ranged interparticle attractions. The resulting spatial correlations among facilitated and unfacilitated regions give rise to new relaxation mechanisms that account for non-monotonic dependence of relaxation times on attraction strength as well as logarithmic decay of density correlations in time. These unusual features are a simple consequence of spatial segregation of kinetic constraints, suggesting an alternative physical perspective on attractive colloids than that suggested by mode-coupling theory. Based on the behavior of our model, we predict a crossover from super-Arrhenius to Arrhenius temperature dependence as attractions become dominant at fixed packing fraction.

cond-mat.stat-mech↗

Supercooled Liquids Under Shear: Theory and Simulation

We analyze the behavior of supercooled fluids under shear both theoretically and numerically. Theoretically, we generalize the mode-coupling theory of supercooled fluids to systems under stationary shear flow. Our starting point is the set of generalized fluctuating hydrodynamic equations with a convection term. A nonlinear integro-differential equation for the intermediate scattering function is constructed. This theory is applied to a two-dimensional colloidal suspension. The shear rate dependence of the intermediate scattering function and the shear viscosity is analyzed. We have also performed extensive numerical simulations of a two-dimensional binary liquid with soft-core interactions near, but above, the glass transition temperature. Both theoretical and numerical results show: (i) A drastic reduction of the structural relaxation time and the shear viscosity due to shear. Both the structural relaxation time and the viscosity decrease as $\dotγ^{-ν}$ with an exponent $ν\leq 1$, where $\dotγ$ is the shear rate. (ii) Almost isotropic dynamics regardless of the strength of the anisotropic shear flow.

cond-mat.soft↗

Numerical Investigation of the Entropy Crisis in Model Glass Formers

We investigate numerically the low temperature equilibration of glassy systems via non-local Monte Carlo methods. We re-examine several systems that have been studied previously and investigate new systems in order to test the performance of such methods near the putative Kauzmann temperature, $T_K$, where the configurational entropy is presumed to vanish. Our results suggest that previous numerical claims in favor of and against a thermodynamic transition at a finite $T_K$ must be re-evaluated. Our work provides some guidelines and suggestions for future numerical investigations of disordered systems at high densities and low temperatures.

cond-mat.soft↗

Supercooled Liquids under Shear: Computational Approach

We have performed molecular dynamics simulations for a model two-dimensional soft-core mixture in a supercooled state. The mixture exhibits a slow structural relaxation in a quiescent state, however, the relaxation is much enhanced in sheared states. There observed surprisingly small anisotropy both in the coherent and incoherent density correlation functions even under extremely strong shear which is $10^3$ times faster than the structural relaxation rate. The present simulation results agree well with predictions of the recently developed mode-coupling theory in shear.

cond-mat.soft↗

Supercooled liquids under shear: A mode-coupling theory approach

We generalize the mode-coupling theory of supercooled fluids to systems under stationary shear flow. Our starting point is the generalized fluctuating hydrodynamic equations with a convection term. The method is applied to a two dimensional colloidal suspension. The shear rate dependence of the intermediate scattering function and shear viscosity is analyzed. The results show a drastic reduction of the structural relaxation time due to shear and strong shear thinning behavior of the viscosity which are in qualitative agreement with recent simulations. The microscopic theory with minimal assumptions can explain the behavior far beyond the linear response regime.

cond-mat.soft↗

A Fully Self-Consistent Treatment of Collective Fluctuations in Quantum Liquids

The problem of calculating collective density fluctuations in quantum liquids is revisited. A fully quantum mechanical self-consistent treatment based on a quantum mode-coupling theory [E. Rabani and D.R. Reichman, J. Chem. Phys.116, 6271 (2002)] is presented. The theory is compared with the maximum entropy analytic continuation approach and with available experimental results. The quantum mode-coupling theory provides semi-quantitative results for both short and long time dynamics. The proper description of long time phenomena is important in future study of problems related to the physics of glassy quantum systems, and to the study of collective fluctuations in Bose fluids.

cond-mat.stat-mech↗

Mean-Field Theory, Mode-Coupling Theory, and the Onset Temperature in Supercooled Liquids

We consider the relationship between the temperature at which averaged energy landscape properties change sharply ($T_{o}$), and the breakdown of mean-field treatments of the dynamics of supercooled liquids. First, we show that the solution of the wavevector dependent mode-coupling equations undergoes an ergodic-nonergodic transition consistently close to $T_{o}$. Generalizing the landscape concept to include hard-sphere systems, we show that the property of inherent structures that changes near $T_{o}$ is governed more fundamentally by packing and free volume than potential energy. Lastly, we study the finite-size Random Orthogonal Model (ROM), and show that the onset of noticeable corrections to mean-field behavior occurs at $T_{o}$. These results highlight new connections between the energy landscape and mode-coupling approach to supercooled liquids, and identify what features of the relaxation of supercooled liquids are properly captured by mode-coupling theory.

cond-mat.soft↗

The nature of slow dynamics in a minimal model of frustration-limited domains

We present simulation results for the dynamics of a schematic model based on the frustration-limited domain picture of glass-forming liquids. These results are compared with approximate theoretical predictions analogous to those commonly used for supercooled liquid dynamics. Although model relaxation times increase by several orders of magnitude in a non-Arrhenius manner as a microphase separation transition is approached, the slow relaxation is in many ways dissimilar to that of a liquid. In particular, structural relaxation is nearly exponential in time at each wave vector, indicating that the mode coupling effects dominating liquid relaxation are comparatively weak within this model. Relaxation properties of the model are instead well reproduced by the simplest dynamical extension of a static Hartree approximation. This approach is qualitatively accurate even for temperatures at which the mode coupling approximation predicts loss of ergodicity. These results suggest that the thermodynamically disordered phase of such a minimal model poorly caricatures the slow dynamics of a liquid near its glass transition.

cond-mat.stat-mech↗

A Molecular Hydrodynamic Theory of Supercooled Liquids and Colloidal Suspensions under Shear

We extend the conventional mode-coupling theory of supercooled liquids to systems under stationary shear flow. Starting from generalized fluctuating hydrodynamics, a nonlinear equation for the intermediate scattering function is constructed. We evaluate the solution numerically for a model of a two dimensional colloidal suspension and find that the structural relaxation time decreases as $\dotγ^{-ν}$ with an exponent $ν\leq 1$, where $\dotγ$ is the shear rate. The results are in qualitative agreement with recent molecular dynamics simulations. We discuss the physical implications of the results.

cond-mat.stat-mech↗

Trap Model and Slow Dynamics in Supercooled Liquids

The predictions of a class of phenomenological trap models of supercooled liquids are tested via computer simulation of a model glass-forming liquid. It is found that a model with a Gaussian distribution of trap energies provides a good description of the landscape dynamics, even at temperatures above $T_{c}$, the critical temperature of mode-coupling theory. A scenario is discussed whereby deep traps are composed of collections of inherent structures above $T_{c}$ and single inherent structures below $T_{c}$. Deviations from the simple Gaussian trap picture are quantified and discussed.

cond-mat.soft↗

Spectral diffusion on ultralong time scales in low temperature glasses

A dynamical theory is constructed to describe spectral diffusion in glasses in the temperature range near 1 Kelvin on long time scales. The theory invokes interacting tunneling centers (TLS) which provide an excess contribution to the spectral hole width which qualitatively accounts for the deviation from standard logarithmic line broadening observed by Maier et al. [Phys. Rev. Lett. 76, 2085 (1996)]. Alternative explanation schemes of the nonlogarithmic line broadening, avoiding interacting TLS, are discussed. We devise experimental tests which could be used to access the validity of the proposed theories.

cond-mat↗

Some comments on the nature of universal properties in low-temperature glasses

We discuss the recent theory of Burin and Kagan that attempts to explain the existence of universal low temperature properties in amorphous solids. We suggest a realistic experimental scenario that could be used to test the theory. We comment on the results of an experiment that has already been performed in the proposed geometry.

cond-mat↗