Filming movies of attosecond charge migration in single molecules with high harmonic spectroscopy

Lixin He, Siqi Sun, Pengfei Lan (), Yanqing He, Bincheng Wang, Pu Wang, Xiaosong Zhu, Liang Li, Wei Cao, Peixiang Lu () and C. D. Lin
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Lixin He: Huazhong University of Science and Technology
Siqi Sun: Huazhong University of Science and Technology
Pengfei Lan: Huazhong University of Science and Technology
Yanqing He: Huazhong University of Science and Technology
Bincheng Wang: Huazhong University of Science and Technology
Pu Wang: Huazhong University of Science and Technology
Xiaosong Zhu: Huazhong University of Science and Technology
Liang Li: Huazhong University of Science and Technology
Wei Cao: Huazhong University of Science and Technology
Peixiang Lu: Huazhong University of Science and Technology
C. D. Lin: Kansas State University

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract Electron migration in molecules is the progenitor of chemical reactions and biological functions after light-matter interaction. Following this ultrafast dynamics, however, has been an enduring endeavor. Here we demonstrate that, by using machine learning algorithm to analyze high-order harmonics generated by two-color laser pulses, we are able to retrieve the complex amplitudes and phases of harmonics of single fixed-in-space molecules. These complex dipoles enable us to construct movies of laser-driven electron migration after tunnel ionization of N2 and CO2 molecules at time steps of 50 attoseconds. Moreover, the angular dependence of the migration dynamics is fully resolved. By examining the movies, we observe that electron holes do not just migrate along the laser polarization direction, but may swirl around the atom centers. Our result establishes a general scheme for studying ultrafast electron dynamics in molecules, paving a way for further advance in tracing and controlling photochemical reactions by femtosecond lasers.

Date: 2022
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DOI: 10.1038/s41467-022-32313-0

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