Correlation of structure and mechanical response in solid-like polymers

Employing large scale molecular dynamics simulations, we measure the uniaxial tensile response of amorphous and semicrystalline states of a coarse-grained PVA bead-spring model. The response beyond the elastic limit encompasses strain-softening and strain-hardening regimes. To understand the underlying mechanisms of plastic deformation, we analyse conformational and structural changes of polymers. In particular, we characterise the volume distribution of crystalline domains along the stress–strain curve. The strain-softening regime in semicrystalline samples is dominated by deformation of crystalline parts, while strain-hardening involves unfolding and alignment of chains in both amorphous and crystalline parts. Comparing the tensile response of semicrystalline and amorphous polymers, we find similar conformations of polymers for both systems in the strain-hardening regime.