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<p>Manipulating intramolecular electron transportation can fundamentally modulate the optical property, electromagnetic behavior and chemical reactivity of molecules. Achieving simultaneous control of multiple ( ≥2) transport pathways within a single molecule, however, remains a significant challenge. Herein, we report light-gated modulation of two distinct conductive pathways in single donor-acceptor Stenhouse adduct (DASA) molecules using the scanning tunneling microscopy break-junction (STM-BJ) technique. The donor and π-bridge pathways are separately controlled by designing DASAs with two thiomethyl anchoring sites. In the donor pathway, a side-chain modulation mechanism operates, where <i>linear</i>-to-<i>cyclic</i> isomerization induces electronic redistribution and increases the conductivity. In contrast, the π-bridge pathway is governed by a main-chain modulation mechanism, in which deformation of the π-conjugated backbone decreases the conductivity. By synthesizing DASAs containing three thiomethyl anchoring sites, these two conductive pathways are integrated within a single-molecule junction and can be simultaneously modulated under 635 nm red-light irradiation and dark relaxation. The π-bridge transport in the <i>linear</i> state exhibits mixed through-bond and through-space character, while photoisomerization leads to an increased through-space contribution in the <i>cyclic</i> state driven by cyclopentenone formation. These results highlight DASAs’ potential in understanding molecular electronics and developing photoresponsive molecular-scale devices.</p>

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Photogated two conductive pathways of donor-acceptor Stenhouse adducts in single-molecule junctions

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月16日

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  • Fanxi Sun,
  • Shengqing Jiang,
  • Hanjun Zhang,
  • Rui Wang,
  • Yu Ji,
  • Songjun Hou,
  • Maolin Zhang,
  • Gaolu Zhu,
  • Tianfang Shi,
  • Jiayu Li,
  • Yuantao Zheng,
  • Wenshu Liu,
  • Yangyang Pan,
  • Hao Luo,
  • Xu Deng,
  • Yonghao Zheng,
  • Chen Wei,
  • Dongsheng Wang

摘要

Manipulating intramolecular electron transportation can fundamentally modulate the optical property, electromagnetic behavior and chemical reactivity of molecules. Achieving simultaneous control of multiple ( ≥2) transport pathways within a single molecule, however, remains a significant challenge. Herein, we report light-gated modulation of two distinct conductive pathways in single donor-acceptor Stenhouse adduct (DASA) molecules using the scanning tunneling microscopy break-junction (STM-BJ) technique. The donor and π-bridge pathways are separately controlled by designing DASAs with two thiomethyl anchoring sites. In the donor pathway, a side-chain modulation mechanism operates, where linear-to-cyclic isomerization induces electronic redistribution and increases the conductivity. In contrast, the π-bridge pathway is governed by a main-chain modulation mechanism, in which deformation of the π-conjugated backbone decreases the conductivity. By synthesizing DASAs containing three thiomethyl anchoring sites, these two conductive pathways are integrated within a single-molecule junction and can be simultaneously modulated under 635 nm red-light irradiation and dark relaxation. The π-bridge transport in the linear state exhibits mixed through-bond and through-space character, while photoisomerization leads to an increased through-space contribution in the cyclic state driven by cyclopentenone formation. These results highlight DASAs’ potential in understanding molecular electronics and developing photoresponsive molecular-scale devices.