Plastic deformation of the stack
of alternating crystal and amorphous
layers typical of semicrystalline polyethylene is studied by molecular
dynamics simulation. A previous investigation of the semicrystalline
layered stack undergoing isochoric extension is extended here to include several new modes of deformation: isostress
extension, isostress compression, and isochoric shear, at 350 K and
deformation rates of 5 × 107 and 5 × 106 s–1. The observed stress–strain responses
are interpreted in terms of the underlying structural evolution of
the material for each mode of deformation. Under tensile deformation,
crystallographic slip was observed at low strains (0 < e
3 < 0.08) regardless of deformation rate.
Different yield mechanisms were observed for the different deformation
rates. To explain the response at intermediate strains (0.08 < e
3 < 0.26), we introduce the concept of “bridging
entanglements”, which are temporary, physical bridges between
crystal lamellae comprising entanglements involving chain segments
belonging to different crystal lamellae. At high strains (e
3 > 0.26), melting and recrystallization
were
observed at the slower deformation rate, while surface melting and
cavitation were observed at the faster deformation rate. Under compressive
deformation at the slower deformation rate, crystallographic slip
was again observed at low strains. For the faster compressive deformation,
an initial period of rapid stress growth at low strain was observed.
This initial stress growth then transitions to a process of fine crystallographic
slip at a strain of e
3 = −0.005.
At intermediate strains under compressive deformation, the release
of bridging entanglements is observed for both strain rates. However,
no melting or recrystallization phenomena were observed under compression,
even at the highest strains simulated (e
3 = −0.33). Under shear deformation, interlamellar slip was
observed for both zx and zy shear
(strain gradient parallel to stacking direction). Chain segments tend
to stretch and align in the shear direction. Interestingly, under
shear deformation this semicrystalline polyethylene exhibits transient
behavior typical of non-Newtonian fluids.