The effect of the topology of the amorphous phase and phase interconnectivity on the stability of the deformation of semicrystalline polyethylene was investigated. The chain topology was modified by crosslinking the samples with electron beam irradiation. The samples were deformed by plane-strain compression, while the accompanying structural changes were monitored with X-ray and differential scanning calorimetry (DSC). At the true strain around of e = 0.3, the lamellar stacks parallel to the loading direction experienced microbuckling instability, which shortly led to the cooperative kinking of lamellae. Macroscopically, this showed up as the ‘second yield.’ Buckling is driven by the different stiffness levels of the hard and soft layers and their strong connectivity—for given layer thickness, the critical strain for buckling appeared proportional to the stiffness of the amorphous phase. Above e = 1.0, lamellae fragmentation was observed. This resulted from the localization of crystallographic slip, which was triggered by stress concentrations generated at lamellae faces by taut ‘stress transmitter’ (ST) chains. Accordingly, the fragmentation was found to be dependent on the surface fraction of STs at the amorphous-crystal interface: a low concentration of STs resulted in fewer but stronger stress concentrations, which led to earlier slip localization, followed quickly by lamellae fragmentation. The observed instabilities, either lamellae kinking or fragmentation, profoundly influenced the deformation process as well as the resultant structure. Both phenomena relieved much of the structural constraints imposed on deforming lamellae and make further strain accommodation easier.
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