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<p>Light is a powerful stimulus for regulating molecular functions, yet achieving precise and efficient photoswitching remains a significant challenge in organic materials, particularly in the aggregate state. Here we report a strategy based on dynamic through-space conjugation (TSC) to regulate photoswitching in Schiff-base crystals. Upon photoexcitation, the system undergoes an excited-state intramolecular proton transfer followed sequentially by <i>cis</i>-<i>trans</i> keto isomerization, a process in which electrons near the nitrogen atom dynamically couple with adjacent π-donors. This transient nitrogen-based TSC, captured by the femtosecond transient absorption spectroscopy and corroborated by high-pressure experiments and calculations, modulates both the transition-state barrier and the stability of the metastable state, thereby markedly enhancing photoswitching efficiency. Beyond mechanistic insight, this study introduces a design paradigm that exploits dynamic nitrogen-based TSC to engineer light-driven logic devices, with broad implications extending from artificial vision sensors to molecular motors.</p>

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Tunable photofluorochromic switch driven by dynamic through-space conjugation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年7月30日

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  • Zuping Xiong,
  • Jianyu Zhang,
  • Qian Li,
  • Xiong Liu,
  • Yanan Wang,
  • Xiang Li,
  • Zhaosheng Qian,
  • Jing Zhi Sun,
  • Ben Zhong Tang,
  • Haoke Zhang

摘要

Light is a powerful stimulus for regulating molecular functions, yet achieving precise and efficient photoswitching remains a significant challenge in organic materials, particularly in the aggregate state. Here we report a strategy based on dynamic through-space conjugation (TSC) to regulate photoswitching in Schiff-base crystals. Upon photoexcitation, the system undergoes an excited-state intramolecular proton transfer followed sequentially by cis-trans keto isomerization, a process in which electrons near the nitrogen atom dynamically couple with adjacent π-donors. This transient nitrogen-based TSC, captured by the femtosecond transient absorption spectroscopy and corroborated by high-pressure experiments and calculations, modulates both the transition-state barrier and the stability of the metastable state, thereby markedly enhancing photoswitching efficiency. Beyond mechanistic insight, this study introduces a design paradigm that exploits dynamic nitrogen-based TSC to engineer light-driven logic devices, with broad implications extending from artificial vision sensors to molecular motors.