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

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 lase

SUBMITTER: He L 

PROVIDER: S-EPMC9357086 | biostudies-literature | 2022 Aug

REPOSITORIES: biostudies-literature