Entanglements in strongly strained high molecular weight polymer melts

We study highly entangled, fully equilibrated polymer melts [1] subject to strong isochoric uniaxial deformation in the non-linear viscoelastic regime by extensive molecular dynamics simulations. It is shown that the over-all conformations of the original paths as well as the primitive paths (PPs) affinely follow the deformation, while the distribution of entanglements along the PPs does not [2]. The signature of chain retraction predicted by the tube model right after deformation is verified qualitatively but not quantitatively in all directions [3]. Upon further relaxation an inhomogeneous distribution of topological constraints in the melts due to long-lived clustering of entanglements and the delayed relaxation in chain conformation is observed.

[1] H.-P. Hsu and K. Kremer, J. Chem. Phys. 144, 154907 (2016)
[2] H.-P. Hsu and K. Kremer, ACS Macro Lett. 7, 107 (2018)
[3] H.-P. Hsu and K. Kremer. Phys. Rev. Lett. 121, 167801 (2018)