Relaxation times obtained from the bond autocorrelation function for the pure polymer (×) and the antiplasticizer (엯). The solid lines are fits of high-temperature results using Eq. (4) the Arrhenius equation. Approximate values of are indicated in the figure; the dashed lines indicate a fit to Eq. (6). The inset shows fits of using Eq. (3).
Shear modulus for the pure polymer and the polymer/antiplasticizer mixture. The inset shows the density of each system as a function of temperature.
Probability of finding a string of length for the pure polymer (◇) and the antiplasticized system (엯). The solid and dashed lines are for and 1.40, respectively. The inset shows the degree of cooperativity of the strings for each system as a function of temperature.
Mean string length at different temperatures for the pure polymer (◇) and the antiplasticized system (엯). The inset shows the average composition (mole fraction) of the strings with a length greater than one for the antiplasticized system. The bulk value of is 0.296.
Probability of finding a monomer with a given Voronoi volume averaged over all particles in the 13 configurations (solid line, see text) and for the mobile particles (dashed line).
Probability of finding a monomer with a given tetrahedricity averaged over all particles (solid line) and the mobile particles (dashed line).
Main figure: Probability of finding a particle with a given propensity for the antiplasticized system. The distribution for the antiplasticized polymer monomers are shown in the solid line and antiplasticizer particles in the dashed line. Inset: Probability distribution of for the pure polymer system (solid line) and the antiplasticized system (dashed line).
Change in the propensity distribution with mobility. The distributions for the pure polymer system (◇) and antiplasticized system (엯) are shown. The distribution is averaged over all particles in the solid lines, and only the mobile particles in the dashed lines.
(Color) Local propensities in the pure polymer (top) and the antiplasticized system (bottom). Length scales are in units of , and the propensity values are averaged over local cubes with sides of length . Note that the scale is different on each color bar, with the range larger on the antiplasticized case.
Fragility parameter and ratios of the characteristic temperatures for the pure polymer (PP) and antiplasticized polymer (AP) system. Also included are values of the same ratios from Ref. 11 for the fragile (FS) and strong (FF) glass-forming polymers with a molecular mass . The run-to-run variation of the numerical estimates shown here and in the text of the paper is less than 2%.
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