Parameter-free predictions of the viscoelastic response of glassy polymers from non-affine lattice dynamics

Soft Matter
Vladimir V PalyulinAlessio Zaccone

Abstract

We study the viscoelastic response of amorphous polymers using theory and simulations. By accounting for internal stresses and considering instantaneous normal modes (INMs) within athermal non-affine theory, we make parameter-free predictions of the dynamic viscoelastic moduli obtained in coarse-grained simulations of polymer glasses at non-zero temperatures. The theoretical results show very good correspondence with rheology data collected from molecular dynamics simulations over five orders of magnitude in frequency, with some instabilities that accumulate in the low-frequency part on approach to the glass transition. These results provide evidence that the mechanical glass transition itself is continuous and thus represents a crossover rather than a true phase transition. The relatively sharp drop of the low-frequency storage modulus across the glass transition temperature can be explained mechanistically within the proposed theory: the proliferation of low-eigenfrequency vibrational excitations (boson peak and nearly-zero energy excitations) is directly responsible for the rapid growth of a negative non-affine contribution to the storage modulus.

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Citations

Jan 22, 2020·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Alessio Zaccone
Jul 23, 2020·Soft Matter·Masanari ShimadaAtsushi Ikeda
Sep 10, 2020·Soft Matter·Céline Ruscher, Jörg Rottler
Dec 16, 2019·The Journal of Chemical Physics·Bingyu CuiDavid Rodney
May 6, 2019·Physical Review Letters·Matteo Baggioli, Alessio Zaccone
Jan 23, 2020·Physical Review. E·Prasenjit DasItamar Procaccia
Aug 5, 2020·Proceedings of the National Academy of Sciences of the United States of America·Alessio Zaccone, Kostya Trachenko
Jan 27, 2021·Proceedings of the National Academy of Sciences of the United States of America·Alessio Zaccone, Matteo Baggioli
May 20, 2021·Physical Review. E·D A Conyuh, Y M Beltukov
Jan 5, 2021·The Journal of Physical Chemistry Letters·Alessio Zaccone, Laurence Noirez

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Methods Mentioned

BETA
mechanical spectroscopy
neutron inelastic scattering

Software Mentioned

LAMMPS

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