We found a match
Your institution may have access to this item. Find your institution then sign in to continue.
- Title
Filming movies of attosecond charge migration in single molecules with high harmonic spectroscopy.
- Authors
He, Lixin; Sun, Siqi; Lan, Pengfei; He, Yanqing; Wang, Bincheng; Wang, Pu; Zhu, Xiaosong; Li, Liang; Cao, Wei; Lu, Peixiang; Lin, C. D.
- 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. Seeing molecules in action under the influence of very short pulses is interesting. Here the authors demonstrate charge migration dynamics in molecules by using high harmonic spectroscopy and machine learning algorithm.
- Subjects
SINGLE molecules; ATTOSECOND pulses; LASER pulses; MACHINE learning; SPECTROMETRY; CHEMICAL reactions; FEMTOSECOND lasers
- Publication
Nature Communications, 2022, Vol 13, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-022-32313-0