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The orientation behavior of isotactic polypropylene (iPP) in ␣and ␤-crystal form was investigated by rheo-optical Fourier transformed infrared (FTIR) spectroscopy. This method enabled quantification of the degree of orientation as a feature of structural changes during uniaxial elongation in not only the crystalline phase but also the amorphous one. Molecular orientation mechanisms can be successfully derived from experimental results. Generally, three mechanisms were detected for iPP: (1) interlamellar separation in the amorphous phase, (2) interlamellar slip and lamellar twisting at small elongations, and (3) intralamellar slip at high elongations. The third mechanism was favored by ␣-PP, whereas ␤-PP favored the second mechanism, which, in fact, was responsible for the different mechanical properties of both materials at the macroscopic level. On the other hand, crystallization conditions may have significantly affected the amorphous orientation. Nevertheless, for both iPP types the chains in the amorphous phase always oriented less than did those in the crystalline phase. © 2004 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 42: 4478 -4488, 2004

The correlation between the molecular architecture, morphology, and micromechanical deformation behaviour of styrene/butadiene (SB) block copolymers with different architectures (linear and star block copolymers, total styrene content, ΦST = 0.74) was studied using dynamic mechanical analysis (DMA), uniaxial tensile testing, scanning force microscopy (SFM), and high voltage electron microscopy (HVEM). Deformation of the individual phases under uniaxial strain at the molecular level was monitored by Fourier transform infrared (FT‐IR) spectroscopy. It was demonstrated that the morphology and deformation behaviour of these block copolymers are strongly influenced by their molecular topology, block symmetry, and the nature of the interface between the component blocks. While the cylindrical morphology (hexagonal polybutadiene (PB) cylinders in polystyrene (PS) matrix) was observed in a symmetric SBS triblock copolymer with ΦST = 0.74, a “two‐component three‐phase” morphology was found in an asymmetric star block copolymer having an equivalent chemical composition and an SBS arm structure. Likewise, an SBS triblock copolymer with a composition identical to the former ones but with highly asymmetric PS end blocks revealed a lamellar morphology. While no locally confined deformation zones were observed in the lamellar block copolymers, the cylindrical block copolymer was found to deform through the formation of highly localised craze‐like deformation zones.

Summary: The morphology and tensile deformation behaviour of a highly asymmetric styrene/butadiene star block copolymer (polystyrene (PS) content = 74%) containing random PS‐co‐PB (polybutadiene) copolymer as a rubbery phase were investigated. The existence of double yielding, similar to that observed in some semicrystalline polymers, was detected in this nanostructured amorphous polymer. The observed phenomenon may be correlated with two different micromechanical processes taking place at the initial stage of deformation.The stress‐strain curve of the star block copolymer prepared here (each curve represents a different method). The two yield points are clearly visible (labelled I and II).imageThe stress‐strain curve of the star block copolymer prepared here (each curve represents a different method). The two yield points are clearly visible (labelled I and II).