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Volumn 60, Issue 5, 1999, Pages 5714-5724

Dynamic entropy as a measure of caging and persistent particle motion in supercooled liquids

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[No Author keywords available]

Indexed keywords

ARTICLE;

EID: 0001403846     PISSN: 1063651X     EISSN: None     Source Type: Journal    
DOI: 10.1103/PhysRevE.60.5714     Document Type: Article
Times cited : (72)

References (116)
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    • this reference the authors introduced an energy metric to quantify the time scale over which effective ergodicity is achieved in simulations
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    • The maximum Lyapunov exponent is aproximately proportional to (Formula presented) 1420
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    • since (Formula presented) 14 for Brownian motion. The extension of dynamic entropy to the scale dependent quantity (Formula presented) resolves this unsatisfactory situation
    • The existence of a finite, positive (Formula presented) is often taken as a defining characteristic of “chaos” in a dynamical system, but this definition excludes Brownian motion, the prototypical model of chaotic motion in molecular physics [N. Wiener, Am. J. Math. 60, 897 (1938)] since (Formula presented) 14 for Brownian motion. The extension of dynamic entropy to the scale dependent quantity (Formula presented) resolves this unsatisfactory situation.
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    • This work has stimulated the investigation of local escape rates as a measure of particle mobilities in cooled liquids [B. Reardon and J. Kieffer (unpublished)]
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    • Previous work identifying instances of stringlike collective motion in simulations of supercooled liquids includes J. L. Barrat, J. N. Roux, and J. P. Hansen, Chem. Phys. 149, 197 (1990)
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    • The Lennard-Jones interaction parameters (Formula presented) and (Formula presented) are given by (Formula presented) (Formula presented) (Formula presented) (Formula presented) (Formula presented) and (Formula presented) Lengths are defined in units of (Formula presented) temperature (Formula presented) in units of (Formula presented) and time (Formula presented) in units of (Formula presented)
    • The Lennard-Jones interaction parameters (Formula presented) and (Formula presented) are given by (Formula presented) (Formula presented) (Formula presented) (Formula presented) (Formula presented) and (Formula presented) Lengths are defined in units of (Formula presented) temperature (Formula presented) in units of (Formula presented) and time (Formula presented) in units of (Formula presented)
  • 59
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    • Recall that for this same system simulated along a different path, the same value of (Formula presented) was found from an analysis of the minority (Formula presented) particles only 39
    • Recall that for this same system simulated along a different path, the same value of (Formula presented) was found from an analysis of the minority (Formula presented) particles only 39.
  • 60
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    • Collective effects can thus develop at very short times
    • Equipartition of energy implies that the average square velocity (Formula presented) in Eq. (3.6) is proportional to (Formula presented) where (Formula presented) is the particle mass. The mass in this expression can become renormalized by backflow after a short time (time for a sound wave to propagate an interparticle distance, approximately (Formula presented) in liquid argon) in a compressible liquid [R. Zwanzig and M. Bixon, J. Fluid Mech. 69, 21 (1975)]. Collective effects can thus develop at very short times.
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    • See http://www.ctcms.nist.gov/donati/movie.html.
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    • Decoupling of transport properties in supercooled liquids has been investigated in, e.g., D. Ehlich and H. Sillescu, Macromolecules 23, 1600 (1990)
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    • exhibit a breakdown of the inverse scaling between (Formula presented) and the particle rotational relaxation time (which should scale as (Formula presented) in mode-coupling theory)
    • It is important to note that (Formula presented) scales in inverse proportion to (Formula presented) in mode-coupling theory, and that Eq. (3.11) suggests an important shortcoming of this model. Recent data for (Formula presented) dumbbell particles interacting with the same LJ parameters of the present calculation [S. Kammerer, W. Kob, and R. Shilling, Phys. Rev. E 56, 5450 (1998)] exhibit a breakdown of the inverse scaling between (Formula presented) and the particle rotational relaxation time (which should scale as (Formula presented) in mode-coupling theory).
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    • Kammerer, S.1    Kob, W.2    Shilling, R.3
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    • Recent work has shown that the fraction of unstable shoulder modes for the present LJ model tends to vanish as (Formula presented) [C. Donati et al. (unpublished)]
    • J. Chem. Phys.P. Madden, T. Keyes, and G. Seeley, 94, 6762 (1991).Recent work has shown that the fraction of unstable shoulder modes for the present LJ model tends to vanish as (Formula presented) [C. Donati et al. (unpublished)].
    • (1991) J. Chem. Phys. , vol.94 , pp. 6762
    • Madden, P.1    Keyes, T.2    Seeley, G.3


* 이 정보는 Elsevier사의 SCOPUS DB에서 KISTI가 분석하여 추출한 것입니다.