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Probing tunneling dynamics of dissociative H2 molecules using two-color bicircularly polarized fields

Zhenning Guo1, Yiqi Fang1, Peipei Ge1, Xiaoyang Yu1, Jiguo Wang1, Meng Han1,2, Qihuang Gong1,3,4, and Yunquan Liu1,3,4,*

  • 1State Key Laboratory for Mesoscopic Physics and Frontiers Science Center for Nano-optoelectronics, School of Physics, Peking University, Beijing 100871, China
  • 2Laboratorium für Physikalische Chemie, ETH Zürich, Zürich 8093, Switzerland
  • 3Collaborative Innovation Center of Quantum Matter, Beijing 100871, China
  • 4Collaborative Innovation Center of Extreme Optics, Shanxi University, Taiyuan, Shanxi 030006, China

  • *yunquan.liu@pku.edu.cn

Phys. Rev. A 104, L051101 – Published 2 November, 2021

DOI: https://doi.org/10.1103/PhysRevA.104.L051101

Abstract

Probing and manipulating the electronic motion in the ultrafast laser molecular interaction provides the pathways for quantum imaging and controlling chemical reactions. Recently, the emerging application of attosecond metrology of ultrafast electron dynamics has accessed the time scale of the most fundamental processes in molecular chemical reactions. Here, we probe the tunneling dynamics of internuclear-dependent dissociative reaction of H2 with angular streaking using two-color bicircularly polarized femtosecond laser pulses. By measuring high-resolution photoelectron spectroscopy, we disentangle the orientation and internuclear-distance dependent effect of the long-range Coulomb potential and the initial phase on molecular-frame photoelectron momentum distributions, and stereo extract the phase gradient of the tunneling electron wave packets and Wigner time delay during the dissociative ionization using two-color bicircular fields. The work has an insight into the clocking of ultrafast spatiotemporal photoelectron dynamics and the quantum control of molecular chemical processes via sculptured circular fields, which can be applied to polyatomic molecules.

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