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Monitoring ultrafast vibrational dynamics of isotopic molecules with frequency modulation of high-order harmonics.
Nature Communications ( IF 16.6 ) Pub Date : 2018-03-16 , DOI: 10.1038/s41467-018-03568-3
Lixin He , Qingbin Zhang , Pengfei Lan , Wei Cao , Xiaosong Zhu , Chunyang Zhai , Feng Wang , Wenjing Shi , Muzi Li , Xue-Bin Bian , Peixiang Lu , André D. Bandrauk

Molecules constituted by different isotopes are different in vibrational modes, making it possible to elucidate the mechanism of a chemical reaction via the kinetic isotope effect. However, the real-time observation of the vibrational motion of isotopic nuclei in molecules is still challenging due to its ultrashort time scale. Here we demonstrate a method to monitor the nuclear vibration of isotopic molecules with the frequency modulation of high-order harmonic generation (HHG) during the laser-molecule interaction. In the proof-of-principle experiment, we report a red shift in HHG from H2 and D2. The red shift is ascribed to dominant HHG from the stretched isotopic molecules at the trailing edge of the laser pulse. By utilizing the observed frequency shift, the laser-driven nuclear vibrations of H2 and D2 are retrieved. These findings pave an accessible route toward monitoring the ultrafast nuclear dynamics and even tracing a chemical reaction in real time.

中文翻译:

通过高阶谐波的频率监控来监测同位素分子的超快振动动力学。

由不同的同位素构成的分子在振动模式上是不同的,从而有可能通过动力学同位素效应阐明化学反应的机理。然而,由于其超短的时间尺度,对分子中同位素核振动运动的实时观察仍然具有挑战性。在这里,我们演示了一种在激光-分子相互作用过程中,通过高次谐波产生(HHG)的频率调制来监视同位素分子的核振动的方法。在原理验证实验中,我们报告了HHG从H 2和D 2发生红移。红移归因于来自激光脉冲后缘拉伸同位素分子的主要HHG。通过利用观察到的频移,可以检索H 2和D 2的激光驱动核振动。这些发现为监测超快核动力学甚至实时追踪化学反应铺平了道路。
更新日期:2018-03-16
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