In‐situ Raman spectroscopy analysis to mechanical tests were performed to investigate the deformation micromechanisms of an isotactic polypropylene‐grafted maleic anhydride (PP‐g‐MAH) depending on the crosslinking degree provided by functional polyether amine molecules. The switch from brittle to highly ductile mechanical behaviours was focused in terms of microstructure modifications in real time during stretching. From the Raman spectral analysis, crystallinity index and macromolecular chains orientation factors for both crystalline and amorphous phases were determined. A new orientation factor relative to the polyether segments was proposed. The results shown allow a more complete understanding of the proper micromechanisms of deformation involved in each phase and their interaction between one another. These results also highlight the impact of the crosslinking reaction on the material resilience improvement.
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