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

He, Lixin; Sun, Siqi; Lan, Pengfei; He, Yanqing; Wang, Bincheng; Wang, Pu; Zhu, Xiaosong; Li, Liang; Cao, Wei; Lu, Peixiang; Lin, C. D.

doi:10.1038/s41467-022-32313-0

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

Journal Article · Sat Aug 06 00:00:00 EDT 2022 · Nature Communications

DOI:https://doi.org/10.1038/s41467-022-32313-0· OSTI ID:1904605

He, Lixin ^[1]; Sun, Siqi ^[2];

^[3]; He, Yanqing ^[2]; Wang, Bincheng ^[2]; Wang, Pu ^[2]; Zhu, Xiaosong ^[3]; Li, Liang ^[3];

^[3];

^[4];

^[5]

Huazhong University of Science and Technology, Wuhan (China); Optical Valley Laboratory, Hubei (China)
Huazhong University of Science and Technology, Wuhan (China)
Huazhong University of Science and Technology, Wuhan (China); Optical Valley Laboratory, Hubei (China)
Huazhong University of Science and Technology, Wuhan (China); Optical Valley Laboratory, Hubei (China); CAS Center for Excellence in Ultra-intense Laser Science, Shanghai (China)
Kansas State University, Manhattan, KS (United States)

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.

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Research Organization:: Kansas State Univ., Manhattan, KS (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Key Research and Development Program of China; National Natural Science Foundation of China (NSFC); Natural Science Foundation of Hubei Province

Grant/Contract Number:: FG02-86ER13491; 2019YFA0308300; 2017YFE0116600; 91950202; 12074136; 12021004; 11627809; 11934006; 2021CFB330

OSTI ID:: 1904605

Journal Information:: Nature Communications, Vol. 13, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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