The molecular orientations in the crystalline and the amorphous phases in a quenched
isotactic polypropylene (iPP) film with a smectic structure are studied using an instrument constructed
for simultaneous kinetic measurement of microscopic infrared (MicIR) dichroism from a predetermined
sampling area with a size of 200 × 200 μm2 and macroscopic stress of film uniaxially stretched at a
constant elongation rate at 30 °C. Local deformation behavior in the sampling area is determined for one
sample using a method of photogrammetry. During the passage of the necking through the sampling
area, the local extension ratio λ(t) increases fast from 1.5 to 5, which induces the rapid orientation of iPP
chains in both the crystalline and the amorphous phases. The orientation function of the amorphous
phase, f
am, from the mesoscale deformation of the sampling area is found to be well described by the
pseudo-affine deformation mechanism, since the local area shrinks anisotropically during the passage of
the neck shoulder. The orientation function f
c in the crystalline phase increases linearly with f
am up to
f
am = 0.3 with a slope of 1.85 for all samples tested. In the neck entity, the crystal orientation may lag
behind the amorphous chain orientation due to the enhanced plastic deformations. It is shown that the
behavior of the amorphous phase is essential for the averaged lamellar orientation on the mesoscale.