Zhou Lianrong, Ni Hongcheng, Jiang Zhejun, Qiang Junjie, Jiang Wenyu, Zhang Wenbin, Lu Peifen, Wen Jin, Lin Kang, Zhu Meifang, Dörner Reinhard, Wu Jian
State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai, China.
Collaborative Innovation Center of Extreme Optics, Shanxi University, Taiyuan, China.
Nat Chem. 2023 Sep;15(9):1229-1235. doi: 10.1038/s41557-023-01230-0. Epub 2023 Jun 1.
The light-driven formation of trihydrogen cation has been attracting considerable attention because of its important role as an initiator of chemical reactions in interstellar clouds. To understand the formation dynamics, most previous studies focused on creating H or D from unimolecular reactions of various organic molecules. Here we observe and characterize the ultrafast formation dynamics of D from a bimolecular reaction, using pump-probe experiments that employ ultrashort laser pulses to probe its formation from a D-D dimer. Our molecular dynamics simulations provide an intuitive representation of the reaction dynamics, which agree well with the experimental observation. We also show that the emission direction of D can be controlled using a tailored two-colour femtosecond laser field. The underlying control mechanism is in line with what is known from the light control of electron localization in the bond breaking of single molecules.
由于三氢阳离子在星际云中作为化学反应引发剂的重要作用，光驱动形成三氢阳离子一直备受关注。为了理解其形成动力学，大多数先前的研究集中于通过各种有机分子的单分子反应产生氢或氘。在此，我们利用泵浦 - 探测实验观察并表征了双分子反应中氘的超快形成动力学，该实验使用超短激光脉冲探测其从D - D二聚体的形成过程。我们的分子动力学模拟提供了反应动力学的直观表示，与实验观察结果吻合良好。我们还表明，可以使用定制的双色飞秒激光场来控制氘的发射方向。其潜在的控制机制与单分子键断裂中电子定位的光控制所熟知的情况一致。
