Coarse-grained microscopic model of glass formers

We introduce a coarse-grained model for atomic glass formers. Its elements are physically motivated local microscopic dynamical rules parameterized by observables. Results of the model are established and used to interpret the measured behaviors of supercooled fluids approaching glass transitions. The model predicts the presence of a crossover from hierarchical super-Arrhenius dynamics at short length scales to diffusive Arrhenius dynamics at large length scales. This prediction distinguishes our model from other theories of glass formers and can be tested by experiment.

[1]  H. Sillescu.  Heterogeneity at the glass transition: a review , 1999 .

[2]  O. Yamamuro,et al.  CALORIMETRIC STUDY OF 3-BROMOPENTANE : CORRELATION BETWEEN STRUCTURAL RELAXATION TIME AND CONFIGURATIONAL ENTROPY , 1995 .

[3]  P G Wolynes,et al.  Fragilities of liquids predicted from the random first order transition theory of glasses. , 1999, Proceedings of the National Academy of Sciences of the United States of America.

[4]  Kaori Ito,et al.  Thermodynamic determination of fragility in liquids and a fragile-to-strong liquid transition in water , 1999, Nature.

[5]  P. Harrowell,et al.  A two dimensional glass: microstructure and dynamics of a 2D binary mixture , 1998 .

[6]  C. Angell,et al.  Nonexponential relaxations in strong and fragile glass formers , 1993 .

[7]  Crossover from fragile to strong glassy behavior in kinetically constrained systems. , 2001, Physical review. E, Statistical, nonlinear, and soft matter physics.

[8]  R. Cole,et al.  Approach to glassy behavior of dielectric relaxation in 3‐bromopentane from 298 to 107 K , 1986 .

[9]  C. Angell,et al.  A thermodynamic connection to the fragility of glass-forming liquids , 2001, Nature.

[10]  Steven J. Plimpton,et al.  STRINGLIKE COOPERATIVE MOTION IN A SUPERCOOLED LIQUID , 1998 .

[11]  Pablo G. Debenedetti,et al.  Supercooled liquids and the glass transition , 2001, Nature.

[12]  Gerard T. Barkema,et al.  Monte Carlo Methods in Statistical Physics , 1999 .

[13]  M D Ediger,et al.  Spatially heterogeneous dynamics in supercooled liquids. , 2003, Annual review of physical chemistry.

[14]  C. Angell,et al.  Formation of Glasses from Liquids and Biopolymers , 1995, Science.

[15]  J. Hammersley,et al.  Monte Carlo Methods , 1965 .

[16]  Donald R Uhlmann,et al.  Viscous flow in simple organic liquids , 1972 .

[17]  Glenn H. Fredrickson,et al.  Kinetic Ising model of the glass transition , 1984 .

[18]  Glassy Time-Scale Divergence and Anomalous Coarsening in a Kinetically Constrained Spin Chain , 1999, cond-mat/9904136.

[19]  Boehmer,et al.  Elastic and viscoelastic properties of amorphous selenium and identification of the phase transition between ring and chain structures. , 1993, Physical review. B, Condensed matter.

[20]  David Chandler,et al.  Geometrical explanation and scaling of dynamical heterogeneities in glass forming systems. , 2002, Physical review letters.

[21]  S. Glarum,et al.  Dielectric Relaxation of Isoamyl Bromide , 1960 .

[22]  Peter Sollich,et al.  Glassy dynamics of kinetically constrained models , 2002, cond-mat/0210382.

[23]  Ding-hai Huang,et al.  New insights into the fragility dilemma in liquids , 2001 .

[24]  Baessler,et al.  Viscous flow in supercooled liquids analyzed in terms of transport theory for random media with energetic disorder. , 1987, Physical review letters.

[25]  A. Heuer,et al.  Glass transition : length scales Comparative study of the NMR length scale of dynamic heterogeneities of three different glass formers , 2002 .

[26]  R. Brüning,et al.  A method to determine the kinetics of a supercooled liquid by temperature scanning measurements applied to (Li,Na)acetate and GeO2 , 1999 .

[27]  R. Palmer,et al.  Models of hierarchically constrained dynamics for glassy relaxation , 1984 .

[28]  A. B. Bestul,et al.  Heat Capacity and Thermodynamic Properties of o‐Terphenyl Crystal, Glass, and Liquid , 1972 .

[29]  J. Jäckle,et al.  A hierarchically constrained kinetic Ising model , 1991 .

[30]  P. Viot,et al.  A heterogeneous picture of α relaxation for fragile supercooled liquids , 2000 .

[31]  A. Barlow,et al.  Relaxation in liquids: a defect-diffusion model of viscoelasticity , 1972, Proceedings of the Royal Society of London. A. Mathematical and Physical Sciences.