Multidirectional Angular Electronic Flux during Adiabatic Attosecond Charge Migration in Excited Benzene

Area of Science:

• Quantum Chemistry
• Attosecond Science
• Molecular Dynamics

Background:

• Adiabatic attosecond charge migration (AACM) has been recently observed and simulated.
• Previous studies applied AACM to linear molecules like iodoacetylene cation.
• AACM involves the superposition of ground and excited electronic states.

Purpose of the Study:

• To develop a theory for electronic fluxes during AACM in ring-shaped molecules.
• To apply this theory to oriented benzene prepared in a specific electronic superposition.
• To confirm a previous hypothesis regarding electronic flux patterns in AACM.

Main Methods:

• Developed a modified theory for electronic fluxes, adapting concepts from coherent tunneling.
• Accounted for different timescales, electronic states, and laser pulse preparation.
• Applied the theory to oriented benzene in a superposition of ground and first excited singlet states.

Main Results:

• Observed a multidirectional angular electronic flux in benzene during AACM.
• Identified a distinct 'pincer-motion' type pattern for the electronic flux.
• Quantified the concerted electron flow, finding a maximum of 0.48 electrons.

Conclusions:

• The developed theory successfully describes electronic fluxes during AACM in ring-shaped molecules.
• The 'pincer-motion' flux pattern in benzene is confirmed.
• The study provides a quantitative measure of electron migration dynamics in complex molecular systems.