Summary: The mechanical properties, morphology, and orientation of a poly(dimethylsiloxane) (PDMS) network have been studied during cyclic elongation and recovery by simultaneous Fourier‐transform near‐infrared polarization spectroscopy at temperatures ranging from room temperature to −40 °C. Completely different orientation/recovery mechanisms and changes in the state of order of PDMS were detected as a consequence of cyclic loading/unloading with decreasing temperature. The differences observed at −20 °C compared to room temperature are explained in terms of conformationally regular chain segments, whereas the cooling to −40 °C leads to the formation of lamellar crystals.Stress/strain diagrams of the elongation/recovery‐cycles of the PDMS films.magnified imageStress/strain diagrams of the elongation/recovery‐cycles of the PDMS films.
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