Lin Kang, Hu Xiaoqing, Pan Shengzhe, Chen Fei, Ji Qinying, Zhang Wenbin, Li Hanxiao, Qiang Junjie, Sun Fenghao, Gong Xiaochun, Li Hui, Lu Peifen, Wang Jianguo, Wu Yong, Wu Jian
State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai 200062, China.
Institute of Applied Physics and Computational Mathematics, Beijing 100088, China.
J Phys Chem Lett. 2020 Apr 16;11(8):3129-3135. doi: 10.1021/acs.jpclett.0c00599. Epub 2020 Apr 7.
We experimentally investigate the ultrafast photodissociation dynamics of the SO molecule induced by intense ultrashort laser pulses in a pump-probe scheme. Different three-body fragmentation pathways are discriminated using the time-dependent kinetic energy release spectrum with femtosecond time resolution. A nontrivial three-body fragmentation pathway, denoted as the bonding pathway, is unraveled, in which an intermediate fast rotating O molecule is formed before complete fragmentation. The ultrafast chemical bond rearrangement after electron release is tracked in real time. The bonding pathway generally exists in the three-body fragmentation processes induced by strong laser fields of different wavelengths, which is observed in infrared, ultraviolet, and mixed two-color cases. Our findings are significant for understanding the photon-induced ultrafast processes of the SO molecule in atmospheric chemistry.
我们采用泵浦-探测方案，通过实验研究了强超短激光脉冲诱导的SO分子的超快光解离动力学。利用具有飞秒时间分辨率的含时动能释放谱，区分了不同的三体碎裂途径。揭示了一种非平凡的三体碎裂途径，称为键合途径，即在完全碎裂之前形成一个中间快速旋转的O分子。实时跟踪了电子释放后的超快化学键重排。键合途径通常存在于不同波长强激光场诱导的三体碎裂过程中，在红外、紫外和混合双色情况下均有观察到。我们的研究结果对于理解大气化学中光子诱导的SO分子超快过程具有重要意义。
