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Ultrafast photoinduced C-H bond formation from two small inorganic molecules

Author

Listed:
  • Zhejun Jiang

    (East China Normal University)

  • Hao Huang

    (East China Normal University)

  • Chenxu Lu

    (East China Normal University)

  • Lianrong Zhou

    (East China Normal University)

  • Shengzhe Pan

    (East China Normal University)

  • Junjie Qiang

    (East China Normal University)

  • Menghang Shi

    (East China Normal University)

  • Zhengjun Ye

    (East China Normal University)

  • Peifen Lu

    (East China Normal University)

  • Hongcheng Ni

    (East China Normal University
    Shanxi University)

  • Wenbin Zhang

    (East China Normal University)

  • Jian Wu

    (East China Normal University
    Shanxi University
    Chongqing Institute of East China Normal University
    CAS Center for Excellence in Ultra-intense Laser Science)

Abstract

The formation of carbon-hydrogen (C-H) bonds via the reaction of small inorganic molecules is of great significance for understanding the fundamental transition from inorganic to organic matter, and thus the origin of life. Yet, the detailed mechanism of the C-H bond formation, particularly the time scale and molecular-level control of the dynamics, remain elusive. Here, we investigate the light-induced bimolecular reaction starting from a van der Waals molecular dimer composed of two small inorganic molecules, H2 and CO. Employing reaction microscopy driven by a tailored two-color light field, we identify the pathways leading to C-H photobonding thereby producing HCO+ ions, and achieve coherent control over the reaction dynamics. Using a femtosecond pump-probe scheme, we capture the ultrafast formation time, i.e., 198 ± 16 femtoseconds. The real-time visualization and coherent control of the dynamics contribute to a deeper understanding of the most fundamental bimolecular reactions responsible for C–H bond formation, thus contributing to elucidate the emergence of organic components in the universe.

Suggested Citation

  • Zhejun Jiang & Hao Huang & Chenxu Lu & Lianrong Zhou & Shengzhe Pan & Junjie Qiang & Menghang Shi & Zhengjun Ye & Peifen Lu & Hongcheng Ni & Wenbin Zhang & Jian Wu, 2024. "Ultrafast photoinduced C-H bond formation from two small inorganic molecules," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47137-3
    DOI: 10.1038/s41467-024-47137-3
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    References listed on IDEAS

    as
    1. Zhoulong Fan & Xiangyang Chen & Keita Tanaka & Han Seul Park & Nelson Y. S. Lam & Jonathan J. Wong & K. N. Houk & Jin-Quan Yu, 2022. "Molecular editing of aza-arene C–H bonds by distance, geometry and chirality," Nature, Nature, vol. 610(7930), pages 87-93, October.
    2. Jing Huang & Andrew Quest & Pablo Cruz-Morales & Kai Deng & Jose Henrique Pereira & Devon Cura & Ramu Kakumanu & Edward E. K. Baidoo & Qingyun Dan & Yan Chen & Christopher J. Petzold & Trent R. Northe, 2023. "Complete integration of carbene-transfer chemistry into biosynthesis," Nature, Nature, vol. 617(7960), pages 403-408, May.
    3. Yizhi Xiang & Norbert Kruse, 2016. "Tuning the catalytic CO hydrogenation to straight- and long-chain aldehydes/alcohols and olefins/paraffins," Nature Communications, Nature, vol. 7(1), pages 1-6, December.
    4. Ruijie K. Zhang & Kai Chen & Xiongyi Huang & Lena Wohlschlager & Hans Renata & Frances H. Arnold, 2019. "Enzymatic assembly of carbon–carbon bonds via iron-catalysed sp3 C–H functionalization," Nature, Nature, vol. 565(7737), pages 67-72, January.
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