Thermal Expansion Behavior of the Ordered Domain in Polyimide Films Investigated by Variable Temperature WAXD Measurements

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  • Sekiguchi Keniji
    Department of Chemistry and Materials Science, Tokyo Institute of Technology
  • Takizawa Kazuhiro
    Department of Chemistry and Materials Science, Tokyo Institute of Technology
  • Ando Shinji
    Department of Chemistry and Materials Science, Tokyo Institute of Technology

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Coefficients of thermal expansion (CTEs) along the main chain direction in the ordered domain of aromatic and semi-aliphatic polyimide (PI) films (αc) were determined in order to investigate the thermal expansion behaviors of self-standing PI films in the direction parallel to the film plane. Variable temperature wide-angle X-ray diffraction (VT-WAXD) measurements were performed using a synchrotron radiation facility in the temperature range of 60-360°C. All the PI films showed characteristic WAXD profiles to liquid-crystalline-like ordered domain overlapped with broad and intense amorphous halos, and diffraction peaks corresponding to the repeating unit along the main chain (c-axis) and the inter-chain ordering (Ch-pack) were clearly resolved. The αcs along the c-axis of PIs having rigid-rod structure are negative, whereas those for PIs containing bent linkages, such as ether (-O-) or methylene (-CH2-), in the main chains are large and positive. The αc values coincide well with the in-plane CTEs of the PI films estimated by thermal mechanical analysis (TMA). This indicates that the negative in-plane CTEs observed for the rigid-rod PI films originates from the negative αc in the ordered domain, which originates from the extended main chains with appreciable orientation in the film plane.

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