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Communication: Correlation of the instantaneous and the intermediate-time elasticity with the structural relaxation in glassforming systems
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23.Note that, in principle, the stress tensor may be also written in the molecular representation in terms of the centre of mass position and momentum of the polymeric chain, together with internal parameters Ref. 22. These two representations are hydrodynamically equivalent, e.g., to evaluate transport coefficients. However, there are differences–especially at short times–between the atomic and the molecular stress correlation functions Ref. 22.
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The elastic models of the glass transition relate the increasing solidity of the glassforming systems with the huge slowing down of the structuralrelaxation and the viscous flow. The solidity is quantified in terms of the instantaneous shear modulusG ∞, i.e., the immediate response to a step change in the strain. By molecular-dynamics simulations of a model polymer system, one shows the virtual absence of correlations between the instantaneous elasticity and the structuralrelaxation. Instead, a well-defined scaling is evidenced by considering the elastic response observed at intermediate times after the initial fast stress relaxation. The scaling regime ranges from sluggish states with virtually pure elastic response on the picosecond time scale up to high-mobility states where fast restructuring events are more apparent.
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