journal article·2022-01Open access

Relaxation in non-Markovian models: From static to dynamic heterogeneity

C. Torregrosa Cabanilles, J. Molina-Mateo, R. Sabater i Serra, J.M. Meseguer-Dueñas, J.L. Gómez Ribelles

Abstract

Glass transition processes have often been explained in terms of wide distributions of relaxation times. By means of a simple stochastic model we here show how dynamic heterogeneity is the key to the emergence of the glass transition. A non-Markovian model representing a small open region of the amorphous material was previously shown to reproduce the time and thermal characteristic behavior of supercooled liquids and glasses. Due to the interaction of the open regions with their environment, the temperature dependence of the equilibrium relaxation times differs from the featureless behavior of the relaxation times of closed regions, whose static disorder does not lead to a glass transition, even with wider distributions of equilibrium relaxation times. The dynamic heterogeneity of the open region produces a glass transition between two different regimes: a faster-than-Arrhenius and non-diverging growth of the supercooled liquid relaxation times and an average Arrhenius behavior of the ideal glass. The Kovacs’ expansion gap was studied by evaluating the nonequilibrium distribution of relaxation times after the temperature quenches.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Material Dynamics and Properties · Theoretical and Computational Physics · Liquid Crystal Research Advancements

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (55)

Show source-provided references
1. Perspective: the glass transition10.1063/1.4795539 ↗
2. 50th Anniversary perspective : challenges in the dynamics and kinetics of glass-forming polymers10.1021/acs.macromol.7b01014 ↗
3. Perspective: searching for simplicity rather than universality in glass-forming liquids10.1063/1.5048093 ↗
4. Relationship between the time-domain Kohlrausch-Williams-Watts and frequency-domain Havriliak-Negami relaxation functions10.1103/PhysRevB.44.7306 ↗
5. Local versus global stretched mechanical response in a supercooled liquid near the glass transition10.1103/PhysRevLett.122.105501 ↗
6. Logarithmic moments of relaxation time distributions10.1063/1.1446035 ↗
7. K. Binder (Ed.), Monte Carlo and Molecular Dynamics Simulations in Polymer Science, Oxford University Press, 1995.10.1093/oso/9780195094381.001.0001 ↗
8. The distribution of the relaxation times as seen by bond fluctuation model10.1016/j.polymer.2009.09.039 ↗
9. Transition vitreuse dans les polymeres amorphes: etude phenomenologique10.1007/BFb0050366 ↗
10. Theoretical perspective on the glass transition and amorphous materials10.1103/RevModPhys.83.587 ↗
11. Isobaric volume and enthalpy recovery of glasses. II. A transparent multiparameter theory
12. Relaxation and vibrational properties in metal alloys and other disordered systems10.1088/1361-648X/ab6e41 ↗
13. Spatially heterogeneous dynamics in supercooled liquids10.1146/annurev.physchem.51.1.99 ↗
14. Heterogeneous dynamics in liquids: fluctuations in space and time10.1088/0953-8984/14/23/201 ↗
15. Revealing the link between structural relaxation and dynamic heterogeneity in glass-forming liquids10.1103/PhysRevLett.120.125502 ↗
16. Autonomously revealing hidden local structures in supercooled liquids10.1038/s41467-020-19286-8 ↗
17. Basis glass states: new insights from the potential energy landscape
18. Aspects of non-equilibrium in classical and quantum systems: slow relaxation and glasses, dynamical large deviations, quantum non-ergodicity, and open quantum dynamics10.1016/j.physa.2017.12.149 ↗
19. Non-arrhenius behavior and fragile-to-strong transition of glass-forming liquids10.1103/PhysRevE.101.042131 ↗
20. Cooperativity in the conformational rearrangements of polymer chain segments as seen by bond fluctuation model10.1002/mats.200900008 ↗
21. A simple model for cooperative and non-exponential processes in non-crystalline polymers10.1016/j.jnoncrysol.2010.06.040 ↗
22. Non-Markovian methods in glass transition10.3390/polym12091997 ↗
23. The τ-effective paradox revisited: an extended analysis of Kovacs’ volume recovery data on poly(vinyl acetate)10.1016/S0032-3861(98)00668-5 ↗
24. The τ-effective paradox: new measurements towards a resolution10.1016/j.polymer.2004.11.086 ↗
25. Spatial heterogeneities in structural temperature cause Kovacs’ expansion gap paradox in aging of glasses10.1103/PhysRevLett.124.095501 ↗
26. A topographic view of supercooled liquids and glass formation10.1126/science.267.5206.1935 ↗
27. Exploring the potential energy landscape of glass-forming systems: from inherent structures via metabasins to macroscopic transport
28. Viscous liquids and the glass transition: a potential energy barrier picture10.1063/1.1672587 ↗
29. Properties of a glass-forming system as derived from its potential energy landscape10.1103/PhysRevLett.78.4051 ↗
30. Local energy landscape in a simple liquid10.1103/PhysRevE.90.052307 ↗
31. Energy landscape-driven non-equilibrium evolution of inherent structure in disordered material10.1038/ncomms15417 ↗
32. Structure-property relationships from universal signatures of plasticity in disordered solids10.1126/science.aai8830 ↗
33. Dynamic order-disorder in atomistic models of structural glass formers10.1126/science.1166665 ↗
34. Lattice model of mobility at interfaces: free surfaces, substrates, and bilayers10.1039/c3sm51287h ↗
35. Ross · 2010
36. Rate processes with dynamical disorder10.1021/ar00173a005 ↗
37. Fluctuations of conformational mobility of macromolecules around the glass transition10.1103/PhysRevE.97.062605 ↗
38. Signatures of distinct dynamical regimes in the energy landscape of a glass-forming liquid10.1038/31189 ↗
39. Basic physics of the coupling model: direct experimental evidences10.1021/bk-1997-0676.ch004 ↗
40. Relaxation in liquids, polymers and plastic crystals - strong/fragile patterns and problems10.1016/0022-3093(91)90266-9 ↗
41. Landscape equivalent of the shoving model10.1103/PhysRevE.69.042501 ↗
42. Disentangling interatomic repulsion and anharmonicity in the viscosity and fragility of glasses10.1103/PhysRevB.95.104203 ↗
43. Are polymers standard glass-forming systems? the role of intramolecular barriers on the glass-transition phenomena of glass-forming polymers10.1088/0953-8984/27/10/103101 ↗
44. Corresponding states of structural glass formers10.1021/jp810362g ↗
45. The essentials of the mode-coupling theory for glassy dynamics10.5488/CMP.1.4.873 ↗
46. Effect of disorder on diffusion and viscosity in condensed systems10.1016/0022-3093(88)90396-1 ↗
47. The length of cooperativity at the glass transition in poly(vinyl acetate) from the modeling of the structural relaxation process10.1016/S0032-3861(98)00213-4 ↗
48. Arrhenius-type temperature dependence of the segmental relaxation below Tg10.1063/1.479046 ↗
49. Little evidence for dynamic divergences in ultraviscous molecular liquids10.1038/nphys1033 ↗
50. Using 20-million-year-old amber to test the super-Arrhenius behaviour of glass-forming systems10.1038/ncomms2809 ↗
51. Structural relaxation in a polyester thermoset as seen by thermally stimulated recovery10.1016/S0032-3861(00)00552-8 ↗
52. Departure from the Vogel behaviour in the glass transition - thermally stimulated recovery, creep and dynamic mechanical analysis studies10.1016/j.polymer.2003.04.002 ↗
53. Direct evidence of two equilibration mechanisms in glassy polymers10.1103/PhysRevLett.111.095701 ↗
54. Non-Markovian nonequilibrium information dynamics10.1103/PhysRevE.98.032123 ↗
55. C. Maes, An introduction to the theory of Markov processes mostly for physics students, 2016, (Not published).