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Manipulating Attosecond Charge Migration in Molecules by Optical Cavities.

Yonghao Gu, Bing Gu¹, Shichao Sun

¹Department of Chemistry, Westlake University, Hangzhou 310030, Zhejiang, China.

Journal of the American Chemical Society

|June 30, 2023

Summary

Placing molecules in optical cavities can enhance ultrafast charge migration, a process studied using quantum dynamics. This method allows monitoring of electronic charge movement, revealing localized dynamics within the cavity.

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Area of Science:

Physical Chemistry
Quantum Dynamics
Molecular Spectroscopy

Background:

Charge migration describes ultrafast electronic charge movement in molecules post-photoionization with frozen nuclei.
Understanding charge migration is crucial for controlling molecular electronic behavior.

Purpose of the Study:

To theoretically investigate the quantum dynamics of photoionized 5-bromo-1-pentene.
To explore the induction and enhancement of charge migration using optical cavities.
To examine the collective nature of polaritonic charge migration.

Main Methods:

Theoretical study of quantum dynamics.
Simulation of photoionized 5-bromo-1-pentene within an optical cavity.
Analysis using time-resolved photoelectron spectroscopy principles.

Main Results:

Optical cavities can induce and enhance charge migration in molecules.
Charge migration dynamics in cavities are observed to be local.
Many-molecule collective effects were not observed in cavity-based charge dynamics or polaritonic chemistry.

Conclusions:

Optical cavities offer a method to control and study molecular charge migration.
Cavity-enhanced charge dynamics exhibit localized behavior, distinct from non-cavity spectroscopic observations.
Polaritonic chemistry in cavities does not display significant many-molecule collective effects.