Journal of Chemical Physics
Feedback | Help | Exit
The Journal of Chemical Physics
Search:
   
 
 
 
Next Article
Adsorption of gold on TiC(001): Au–C interactions and charge polarization
High-resolution photoemission and first-principles density-functional slab calculations were used to study the adsorption of gold on a TiC(001) surface. A positive shift in the binding energy of the C...

Decoupling of exchange and persistence times in atomistic models of glass formers

J. Chem. Phys. 127, 211101 (2007); doi:10.1063/1.2803062

Published 3 December 2007

You are not logged in to this journal. Log in

Lester O. Hedges
School of Physics and Astronomy, University of Nottingham, Nottingham NG7 2RD, United Kingdom

Lutz Maibaum and David Chandler
Department of Chemistry, University of California, Berkeley, California 94720-1460, USA

Juan P. Garrahan
School of Physics and Astronomy, University of Nottingham, Nottingham NG7 2RD, United Kingdom
With molecular dynamics simulations of a fluid mixture of classical particles interacting with pairwise additive Weeks-Chandler-Andersen potentials, we consider the time series of particle displacements and thereby determine the distributions for local persistence times and local exchange times. These basic characterizations of glassy dynamics are studied over a range of supercooled conditions and were shown to have behaviors, most notably decoupling, similar to those found in kinetically constrained lattice models of structural glasses. Implications are noted. ©2007 American Institute of Physics
History: Received 15 August 2007; accepted 4 October 2007; published 3 December 2007
Permalink: http://link.aip.org/link/?JCPSA6/127/211101/1
BUY THIS ARTICLE   (US$24)
Download HTML Download Sectioned HTML Download PDF (590 kB) View Cart

KEYWORDS and PACS

Keywords
PACS
  • 61.43.Fs
    Structure of glasses
  • 61.20.Ja
    Computer simulation of liquid structure
  • YEAR: 2007

RELATED DATABASES


To view database links for this article,
you need to log in.
To view database links for this article,
you need to log in.

PUBLICATION DATA

ISSN:
0021-9606 (print)   1089-7690 (online)
Publisher:
AIP is a member of CrossRef AIP

REFERENCES (29)
View in Separate Window/Tab
For access to fully linked references, you need to log in. For access to fully linked references, you need to Log in.
  1. G. H. Fredrickson and H. C. Andersen, Phys. Rev. Lett. 53, 1244 (1984).
  2. F. Ritort and P. Sollich, Adv. Phys. 52, 219 (2003).
  3. J. P. Garrahan and D. Chandler, Phys. Rev. Lett. 89, 035704 (2002).
  4. J. P. Garrahan and D. Chandler, Proc. Natl. Acad. Sci. U.S.A. 100, 9710 (2003).
  5. Y. Jung, J. P. Garrahan, and D. Chandler, Phys. Rev. E 69, 061205 (2004).
  6. Y. Jung, J. P. Garrahan, and D. Chandler, J. Chem. Phys. 123, 084509 (2005).
  7. L. Berthier, D. Chandler, and J. P. Garrahan, Europhys. Lett. 69, 320 (2005).
  8. See, e.g., I. Chang and H. Sillescu, J. Phys. Chem. B 101, 8794 (1997);
    9. S. F. Swallen, P. A. Bonvallet, R. J. McMahon, and M. D. Ediger, Phys. Rev. Lett. 90, 015901 (2003);
    L. Berthier, Phys. Rev. E 69, 020201 (2004);
    S. K. Kumar, G. Szamel, and J. F. Douglas, J. Chem. Phys. 124, 214501 (2006).
  9. For reviews on dynamic heterogeneity see: H. Sillescu, J. Non-Cryst. Solids 243, 81 (1999);
    10. M. D. Ediger, Annu. Rev. Phys. Chem. 51, 99 (2000);
    S. C. Glotzer, J. Non-Cryst. Solids 274, 342 (2000);
    R. Richert, J. Phys.: Condens. Matter 14, R703 (2002);
    H. C. Andersen, Proc. Natl. Acad. Sci. U.S.A. 102, 6686 (2005).
  10. D. Chandler, J. P. Garrahan, R. L. Jack, L. Maibaum, and A. C. Pan, Phys. Rev. E 74, 051501 (2006).
  11. P. Chaudhuri, L. Berthier, and W. Kob, Phys. Rev. Lett. 99, 060604 (2007).
  12. See, for example, E. R. Weeks, J. C. Crocker, A. C. Levitt, A. Schofield, and D. A. Weitz, Science 287, 627 (2000);
    13. V. Prasad, D. Semwogerere, and E. R. Weeks, J. Phys.: Condens. Matter 19, 113102 (2007);
    R. Besseling, E. R. Weeks, A. B. Schofield, and W. C. K. Poon, Phys. Rev. Lett. 99, 028301 (2007);
    Y. Gao and M. L. Kilfoil, ibid. 99, 078301 (2007).
  13. A. C. Pan, J. P. Garrahan, and D. Chandler, Phys. Rev. E 72, 041106 (2005);
    14. A. C. Pan, J. Chem. Phys. 123, 164501 (2005).
  14. The decoupling of the different relevant relaxation rates is also evident from the behavior of four-point dynamic susceptibilities at different length scales, see, for example Refs. 10,15,16.
  15. S. C. Glotzer, V. N. Novikov, and T. B. Schroeder, J. Chem. Phys. 112, 509 (2000).
  16. L. Berthier, G. Biroli, J. P. Bouchaud, W. Kob, K. Miyazaki, and D. Reichman, J. Chem. Phys. 126, 184504 (2007).
  17. L. Maibaum, Ph.D. thesis, University of California Berkeley, 2005.
  18. G. Wahnstrom, Phys. Rev. A 44, 3752 (1991).
  19. See, e.g., N. Lacevic, F. W. Starr, T. B. Schrøder, and S. C. Glotzer, J. Chem. Phys. 119, 7372 (2003);
    20. N. Lacevic and S. C. Glotzer, ibid. 120, 4415 (2004).
  20. J. D. Weeks, D. Chandler, H. C. Andersen, J. Chem. Phys. 54, 5237 (1971).
  21. Molecular dynamics simulations were performed using a microcanonical Verlet algorithm for Fig. 1 and LAMMPS (Ref. 22) for Fig. 2, at temperatures T=5.0–0.36 along a constant density path. The particle numbers and box length, NA=NB=500 and L=9.172 for Fig. 1, and NA=NB=4000 and L=18.344 for Fig. 2, were fixed in each run. The system was prepared at each thermodynamic state point by coupling to a heat bath for time tcool using velocity rescaling or velocity reassigning every 50 time steps. No drift or aging was observed over the equilibration time tequil in thermodynamic or dynamic observables before performing production runs. Both tcool and tequil were significantly longer than the structural relaxation time.
  22. S. J. Plimpton, Large-scale Atomic/Molecular Massively Parallel Simulator (http://lammps.sandia.gov);
    23. S. J. Plimpton, J. Comput. Phys. 117, 1 (1995).
  23. See, e.g., W. Kob and H. C. Andersen, Phys. Rev. E 52, 4134 (1995);
    24. D. N. Perera and P. Harrowell, J. Chem. Phys. 111, 5441 (1999);
    E. Flenner and G. Szamel, Phys. Rev. E 72, 031508 (2005);
    L. Berthier and W. Kob, J. Phys.: Condens. Matter 19, 205130 (2007).
  24. In the context of renewal processes (Ref. 25), exchange and persistence times are called total and excess lifetimes, respectively. If events occur over a very short time scale as compared to waiting times the distributions of persistence and exchange times are related by p(tp)=⟨tx⟩−1[integral]<sub>t[sub p]</sub><sup>[infinity]</sup>p(tx)dtx (Refs. 6,25). In our case, where an event may be built up over time (a displacement of distance d does not occur instantaneously), this relation works only as an approximation. Nevertheless, application of this formula gives reasonable estimates of the behavior.
  25. G. Grimmett and D. Stirzaker, Probability and Random Processes (Oxford University Press, Oxford, 2001).
  26. The distributions of persistence (or first-passage) times for smaller cutoff distances behave differently, see P. Allegrini, J. F. Douglas, and S. C. Glotzer, Phys. Rev. E 60, 5714 (1999). These authors also find that the typical first-passage time for distances comparable to a particle diameter scales with temperature roughly as taualpha, which is consistent with what is expected from dynamic facilitation (Refs. 5,6).
  27. M. Merolle, J. P. Garrahan, and D. Chandler, Proc. Natl. Acad. Sci. U.S.A. 102, 10837 (2005);
    28. J. P. Garrahan, R. L. Jack, V. Lecomte, E. Pitard, K. van Duijvendijk, and F. van Wijland, Phys. Rev. Lett. 98, 195702 (2007).
  28. E. W. Montroll and G. H. Weiss, J. Math. Phys. 6, 167 (1965).
  29. D. A. Stariolo and G. Fabricius, J. Chem. Phys. 125, 064505 (2006).

CITING ARTICLES
For access to citing articles, you need to log in.
For access to citing articles, you need to Log in.


Copyright © American Institute of Physics