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<p>The development of stimuli-responsive switching memory devices and the elucidation of their switching mechanisms in specific environments are crucial for advancing the field of molecular electronics. Herein, we propose two distinct two-dimensional covalent organic frameworks (COFs), namely Py-EDA and Py-BDA, incorporating acetylene (–C≡C–) or diacetylene (–C≡C–C≡C–) moieties, respectively, targeting fabricate memory devices exhibiting stimuli-responsive switching behavior. Our findings demonstrate that the incorporation of acetylene units effectively modulates the electronic band structure and enhances the degree of <i>π</i>-conjugation, resulting in devices that exhibit typical bipolar nonvolatile memory performance. Notably, upon thermal treatment, the memory behavior of the ITO/Py-BDA/Ag device transitions to a write-once-read-many-times (WORM) mode, displaying decreased SET voltage, increased ON/OFF current ratio, and remarkable retention reliability and cycle stability. This switching behavior is attributed to the occurrence of interlayer solid-state topological polymerization at 350 °C, leading to the transformation of diacetylene columnar arrays into enyne chains within Py-BDA, thereby further promoting interlayer charge transfer and separation.</p>

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Thermally triggered topological polymerization in diacetylene-functionalized covalent organic framework toward enhanced memristive properties

  • 期刊论文

  • 发表日期：

    2025年1月3日

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  • Pan-Ke Zhou,
  • Yuxing Huang,
  • Ziyue Yu,
  • Cong Zhang,
  • Qian Chen,
  • Yiping Li,
  • Chao Lin,
  • Xiong Chen

摘要

The development of stimuli-responsive switching memory devices and the elucidation of their switching mechanisms in specific environments are crucial for advancing the field of molecular electronics. Herein, we propose two distinct two-dimensional covalent organic frameworks (COFs), namely Py-EDA and Py-BDA, incorporating acetylene (–C≡C–) or diacetylene (–C≡C–C≡C–) moieties, respectively, targeting fabricate memory devices exhibiting stimuli-responsive switching behavior. Our findings demonstrate that the incorporation of acetylene units effectively modulates the electronic band structure and enhances the degree of π-conjugation, resulting in devices that exhibit typical bipolar nonvolatile memory performance. Notably, upon thermal treatment, the memory behavior of the ITO/Py-BDA/Ag device transitions to a write-once-read-many-times (WORM) mode, displaying decreased SET voltage, increased ON/OFF current ratio, and remarkable retention reliability and cycle stability. This switching behavior is attributed to the occurrence of interlayer solid-state topological polymerization at 350 °C, leading to the transformation of diacetylene columnar arrays into enyne chains within Py-BDA, thereby further promoting interlayer charge transfer and separation.