The excess low-frequency vibrational spectrum, called boson peak, and non-affine elastic response are the most important particularities of glasses. Herein, the vibrational and mechanical properties of polymeric glasses are examined by using coarse-grained molecular dynamics simulations, with particular attention to the effects of the bending rigidity of the polymer chains. As the rigidity increases, the system undergoes a glass transition at a higher temperature (under a constant pressure), which decreases the density of the glass phase. The elastic moduli, which are controlled by the decrease of the density and the increase of the rigidity, show a non-monotonic dependence on the rigidity of the polymer chain that arises from the non-affine component. Moreover, a clear boson peak is observed in the vibrational density of states, which depends on the macroscopic shear modulus G. In particular, the boson peak frequency ωBP is proportional to . These results provide a positive correlation between the boson peak, shear elasticity, and the glass transition temperature.
Amorphous materials exhibit peculiar mechanical and vibrational properties, including non-affine elastic responses and excess vibrational states, i.e., the so-called boson peak (BP). For polymer glasses, these properties are considered to be affected by the bending rigidity of the constituent polymer chains. In our recent work [Tomoshige, et al 2019, Sci. Rep.
9 19514], we have revealed simple relationships between the variations of vibrational properties and the global elastic properties: the response of the BP scales only with that of the global shear modulus. This observation suggests that the spatial heterogeneity of the local shear modulus distribution is insensitive to changes in the bending rigidity. Here, we demonstrate the insensitivity of elastic heterogeneity by directly measuring the local shear modulus distribution. We also study transverse sound wave propagation, which is also shown to scale only with the global shear modulus. Through these analyses, we conclude that the bending rigidity does not alter the spatial heterogeneity of the local shear modulus distribution, which yields vibrational and acoustic properties that are controlled solely by the global shear modulus of a polymer glass.
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