DOI: 10.1126/science.1166665. Dynamic Order-Disorder in Atomistic Models of Structural Glass Formers

Dynamic Order-Disorder in Atomistic Models of Structural Glass Formers

10.1126/science.1166665

Crossref journal-article

American Association for the Advancement of Science (AAAS)

Science (221)

Abstract

The glass transition is the freezing of a liquid into a solid state without evident structural order. Although glassy materials are well characterized experimentally, the existence of a phase transition into the glass state remains controversial. Here, we present numerical evidence for the existence of a novel first-order dynamical phase transition in atomistic models of structural glass formers. In contrast to equilibrium phase transitions, which occur in configuration space, this transition occurs in trajectory space, and it is controlled by variables that drive the system out of equilibrium. Coexistence is established between an ergodic phase with finite relaxation time and a nonergodic phase of immobile molecular configurations. Thus, we connect the glass transition to a true phase transition, offering the possibility of a unified picture of glassy phenomena.

Bibliography

Hedges, L. O., Jack, R. L., Garrahan, J. P., & Chandler, D. (2009). Dynamic Order-Disorder in Atomistic Models of Structural Glass Formers. Science, 323(5919), 1309â1313.

Authors 4

Lester O. Hedges (first)
Robert L. Jack (additional)
Juan P. Garrahan (additional)
David Chandler (additional)

References 31 Referenced 350

10.1021/jp953538d
10.1038/35065704
10.1103/PhysRevLett.66.3020
10.1126/science.287.5453.627
10.1146/annurev.physchem.51.1.99
10.1016/S0022-3093(00)00225-8
10.1073/pnas.0504820102
10.1063/1.2374885
10.1103/PhysRevLett.98.195702
10.1146/annurev.physchem.53.082301.113146
D. Chandler Introduction to Modern Statistical Mechanics (Oxford Univ. Press Oxford 1987).
D. P. Landau K. Binder A Guide to Monte Carlo Simulations in Statistical Physics (Cambridge Univ. Press Cambridge 2000); see section 4.2.3.
10.1103/RevModPhys.57.617
10.1007/s10955-006-9254-0
10.1126/science.1135795
10.1080/0001873031000093582
10.1103/PhysRevLett.73.1376
Supporting materials are available for this article on Science Online.
10.1021/j100303a014
10.1103/PhysRevLett.68.1738
J. P. Hansen I. R. McDonald The Theory of Simple Liquids (Academic Press London 2006).
10.1088/0305-4608/5/5/017
10.1103/PhysRevE.67.031506
10.1103/PhysRevLett.96.057801
10.1103/PhysRevLett.49.1565
10.1088/0034-4885/55/3/001
10.1088/1742-5468/2005/05/P05013
10.1103/PhysRevA.40.1045
10.1063/1.1796231
10.1016/0378-4371(95)00140-3
During the course of this work we have benefited from discussions with T. F. Miller III and F. van Wijland. The work was made possible through grants from the NSF (CHE-0543158 in the early stages for R.J. and D.C. and CHE-0626305 in the later stages for L.H. and D.C.) from the U.S. Office of Naval Research (N00014-07-1-0689 in the late stages for R.J.) and from the Engineering and Physical Sciences Research Council (GR/S54074/01 for J.P.G.).

Dates

Type	When
Created	16 years, 6 months ago (Feb. 6, 2009, 11:48 p.m.)
Deposited	1 year, 7 months ago (Jan. 10, 2024, 4:22 a.m.)
Indexed	20 hours, 57 minutes ago (Aug. 21, 2025, 1:59 p.m.)
Issued	16 years, 5 months ago (March 6, 2009)
Published	16 years, 5 months ago (March 6, 2009)
Published Print	16 years, 5 months ago (March 6, 2009)

Funders 0

None

BibTeX

@article{Hedges_2009, title={Dynamic Order-Disorder in Atomistic Models of Structural Glass Formers}, volume={323}, ISSN={1095-9203}, url={http://dx.doi.org/10.1126/science.1166665}, DOI={10.1126/science.1166665}, number={5919}, journal={Science}, publisher={American Association for the Advancement of Science (AAAS)}, author={Hedges, Lester O. and Jack, Robert L. and Garrahan, Juan P. and Chandler, David}, year={2009}, month=mar, pages={1309–1313} }

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