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Correlation of cooperatively localized rearrangement on the “fluidized domain” in glass substances (or polymers) to their fragility III: Theory of dynamic fragility at isochoric state

Identifieur interne : 000630 ( Main/Exploration ); précédent : 000629; suivant : 000631

Correlation of cooperatively localized rearrangement on the “fluidized domain” in glass substances (or polymers) to their fragility III: Theory of dynamic fragility at isochoric state

Auteurs : Yan Jin [République populaire de Chine] ; Mingshi Song [République populaire de Chine] ; Guixian Hu [République populaire de Chine] ; Daming Wu [République populaire de Chine]

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RBID : ISTEX:1A33DC314579FA856F1797987D1B10DD31F613E2

English descriptors

Abstract

Abstract: A set of universal equations on the reduced stress relaxation modulus with K-W-W stretched exponential function has been derived from the dynamics of α and β structural relaxation processes. In the present work, the K-W-W decay function is used to define the three types of relaxations (single α, single β relaxation and α-β co-relaxation), then their average times of relaxation are theoretically calculated from the reduced shear stress relaxation modulus and the relaxation time spectrum function H(τ). When the average time of co-relaxation, the reference temperatures (ficitive T f and glass transition T g) and the isostructural parameter achieved from the conditions of isostructural glass state are introduced into the reduced shear stress relaxation modulus (G T) under the equilibrium state, a set of correlations between isochoric fragility index (m να, m νβ and m ναβ) and the coupling strength (α and β) under the reference temperatures are derived from the exact definition of isochoric fragility. So the theory of dynamic fragility for glass substances at isochoric state is developed. The theory can predict the following main features of structural relaxations and behavior of isochoric fragility: the temperature dependence of peak relaxation frequency exhibits a bifurcation with a pair of single α and single β relaxations; the temperature dependence of Stickel equation on 1/T exhibits two crossovers with VFTH(1) and VFTH(2) at the temperatures of T f and T g regime; there are two linear correlations between isochoric fragility index (m να and m νβ) and the coupling strength. Fine agreements between the theoretical calculation and experimental results are obtained.

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DOI: 10.1007/s11433-010-4236-2


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<term>Average relaxation time</term>
<term>Average structural relaxation time</term>
<term>Average time</term>
<term>Bifurcation</term>
<term>Bulk modulus</term>
<term>Characteristic time</term>
<term>Chem phys</term>
<term>China phys mech astron</term>
<term>Complex modulus</term>
<term>Compressible</term>
<term>Compressible substance</term>
<term>Conformation fraction</term>
<term>Constituent</term>
<term>Constituent chain</term>
<term>Correlation plot</term>
<term>Crossover</term>
<term>Datum</term>
<term>Decay function</term>
<term>Domain constituent chain</term>
<term>Dynamic equilibrium state</term>
<term>Dynamic fragility</term>
<term>Dynamic fragility index</term>
<term>Empirical equation</term>
<term>Exact definition</term>
<term>Exponential</term>
<term>Exponential function</term>
<term>External stress</term>
<term>Fluidized domain</term>
<term>Fragility</term>
<term>Glass former</term>
<term>Glass substance</term>
<term>Glass transition</term>
<term>In pressure</term>
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<term>Isobaric state</term>
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<term>Linear correlation</term>
<term>Localized rearrangement</term>
<term>Main feature</term>
<term>Mech</term>
<term>Memory effect</term>
<term>Modulus</term>
<term>Ngai</term>
<term>Nonlinearity</term>
<term>Parameter</term>
<term>Phys</term>
<term>Polymer</term>
<term>Primary molecular weight</term>
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<term>Reference temperature</term>
<term>Relaxation</term>
<term>Relaxation stage</term>
<term>Relaxation time</term>
<term>Secondary constituent chain</term>
<term>Shear stress</term>
<term>Shear stress relaxation modulus</term>
<term>Shear stress relaxation modulus curve</term>
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<term>Stress relaxation</term>
<term>Stress relaxation modulus</term>
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<term>Structural process</term>
<term>Structural relaxation</term>
<term>Structural relaxation process</term>
<term>Structural relaxation time</term>
<term>Temperature dependence</term>
<term>Thermal history</term>
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<div type="abstract" xml:lang="en">Abstract: A set of universal equations on the reduced stress relaxation modulus with K-W-W stretched exponential function has been derived from the dynamics of α and β structural relaxation processes. In the present work, the K-W-W decay function is used to define the three types of relaxations (single α, single β relaxation and α-β co-relaxation), then their average times of relaxation are theoretically calculated from the reduced shear stress relaxation modulus and the relaxation time spectrum function H(τ). When the average time of co-relaxation, the reference temperatures (ficitive T f and glass transition T g) and the isostructural parameter achieved from the conditions of isostructural glass state are introduced into the reduced shear stress relaxation modulus (G T) under the equilibrium state, a set of correlations between isochoric fragility index (m να, m νβ and m ναβ) and the coupling strength (α and β) under the reference temperatures are derived from the exact definition of isochoric fragility. So the theory of dynamic fragility for glass substances at isochoric state is developed. The theory can predict the following main features of structural relaxations and behavior of isochoric fragility: the temperature dependence of peak relaxation frequency exhibits a bifurcation with a pair of single α and single β relaxations; the temperature dependence of Stickel equation on 1/T exhibits two crossovers with VFTH(1) and VFTH(2) at the temperatures of T f and T g regime; there are two linear correlations between isochoric fragility index (m να and m νβ) and the coupling strength. Fine agreements between the theoretical calculation and experimental results are obtained.</div>
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