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Approach to the glass transition studied by higher order correlation functions

N Lacević and S C Glotzer

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We present a theoretical framework based on a higher order density correlation function, analogous to that used to investigate spin glasses, to describe dynamical heterogeneities in simulated glass-forming liquids. These higher order correlation functions are a four-point, time-dependent density correlation function g4(r,t) and a corresponding 'structure factor' S4(q,t) which measure the spatial correlations between the local liquid density at two points in space, each at two different times. g4(r,t) and S4(q,t) were extensively studied via molecular dynamics simulations of a binary Lennard-Jones mixture approaching the mode coupling temperature from above in Franz et al (1999 Phil. Mag.  B 79  1827), Donati et al (2002 J. Non-Cryst. Solids  307  215), Glotzer et al (2000 J. Chem. Phys.  112  509), Lacević et al (2002 Phys. Rev.  E 66  030101), Lacević et al (2003 J. Chem. Phys.  submitted) and Lacević (2003 Dissertation  The Johns Hopkins University). Here, we examine the contribution to g4(r,t), S4(q,t) and the corresponding dynamical correlation length, as well as the corresponding order parameter Q(t) and generalized susceptibility χ4(t), from localized particles. We show that the dynamical correlation length ξ4SS(t) of localized particles has a maximum as a function of time t, and the value of the maximum of ξ4SS(t) increases steadily in the temperature range approaching the mode coupling temperature from above.


PACS

64.70.P- Glass transitions of specific systems

61.43.Bn Structural modeling: serial-addition models, computer simulation

Subjects

Condensed matter: structural, mechanical & thermal

Dates

Issue 31 (13 August 2003)

Received 11 June 2003

Published 23 July 2003



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