Jiang Zhejun, Huang Hao, Lu Chenxu, Zhou Lianrong, Pan Shengzhe, Qiang Junjie, Shi Menghang, Ye Zhengjun, Lu Peifen, Ni Hongcheng, Zhang Wenbin, Wu Jian
State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai, 200241, China.
Collaborative Innovation Center of Extreme Optics, Shanxi University, Taiyuan, Shanxi, 030006, China.
Nat Commun. 2024 Apr 2;15(1):2854. doi: 10.1038/s41467-024-47137-3.
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, H 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.
通过小分子无机分子反应形成碳氢键(C-H)对于理解从无机物到有机物的基本转变,进而理解生命起源具有重要意义。然而,C-H键形成的详细机制,特别是动力学的时间尺度和分子水平控制,仍然难以捉摸。在这里,我们从由两个小分子无机物H和CO组成的范德华分子二聚体出发,研究光诱导双分子反应。利用由定制双色光场驱动的反应显微镜,我们确定了导致C-H光键合从而产生HCO离子的途径,并实现了对反应动力学的相干控制。使用飞秒泵浦-探测方案,我们捕捉到了超快形成时间,即198±16飞秒。动力学的实时可视化和相干控制有助于更深入地理解负责C-H键形成的最基本双分子反应,从而有助于阐明宇宙中有机成分的出现。