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<p>The development of polymer dielectrics with extremely low dissipation factors (<i>D</i><sub>f</sub>) in the GHz range is essential for next-generation high-frequency communication and advanced semiconductor technologies. In this study, silicon-containing polyimides (PIs) were systematically synthesized through the incorporation of polysiloxane and double-decker silsesquioxane (DDSQ) units, aiming to elucidate the correlation between molecular structures, higher-order structures, and dielectric properties. Poly(amic acid) precursors were prepared using various tetracarboxylic dianhydrides and silicon-containing diamines, followed by thermal imidization to obtain PI films. Wide-angle X-ray diffraction analysis revealed the formation of periodic layered structures in polysiloxane-containing PIs and the preservation of the cage-like architecture in DDSQ-containing PIs. Dielectric measurements at 10 and 20 GHz demonstrated that the introduction of silicon-containing units reduced the dielectric constant (<i>D</i><sub>k</sub>) to less than 3.0 because of increased free volume. Notably, the <i>D</i><sub>f</sub> values of DDSQ-containing PIs were markedly lower ( ~ 0.002–0.003) than those of polysiloxane-based PIs because of the effective suppression of dipolar orientational polarization originating from the rigid and highly symmetric DDSQ framework. These findings provide an important molecular design strategy for low-loss polymer dielectrics and highlight the potential of DDSQ-based PIs as promising candidates for interlayer insulating materials in high-frequency electronic devices.</p>

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Structure-dielectric property correlations in polysiloxane- and DDSQ-based polyimides measured at high frequencies

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月27日

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  • Erina Yoshida,
  • Natsuko Sashi,
  • Hayato Maeda,
  • Kan Hatakeyama-Sato,
  • Yuta Nabae,
  • Ririka Sawada,
  • Shinji Ando,
  • Teruaki Hayakawa

摘要

The development of polymer dielectrics with extremely low dissipation factors (Df) in the GHz range is essential for next-generation high-frequency communication and advanced semiconductor technologies. In this study, silicon-containing polyimides (PIs) were systematically synthesized through the incorporation of polysiloxane and double-decker silsesquioxane (DDSQ) units, aiming to elucidate the correlation between molecular structures, higher-order structures, and dielectric properties. Poly(amic acid) precursors were prepared using various tetracarboxylic dianhydrides and silicon-containing diamines, followed by thermal imidization to obtain PI films. Wide-angle X-ray diffraction analysis revealed the formation of periodic layered structures in polysiloxane-containing PIs and the preservation of the cage-like architecture in DDSQ-containing PIs. Dielectric measurements at 10 and 20 GHz demonstrated that the introduction of silicon-containing units reduced the dielectric constant (Dk) to less than 3.0 because of increased free volume. Notably, the Df values of DDSQ-containing PIs were markedly lower ( ~ 0.002–0.003) than those of polysiloxane-based PIs because of the effective suppression of dipolar orientational polarization originating from the rigid and highly symmetric DDSQ framework. These findings provide an important molecular design strategy for low-loss polymer dielectrics and highlight the potential of DDSQ-based PIs as promising candidates for interlayer insulating materials in high-frequency electronic devices.