A quantum dynamics method for excited electrons in molecular aggregate system using a group diabatic Fock matrix

Area of Science:

• Computational Chemistry
• Quantum Dynamics
• Molecular Systems

Background:

• Understanding excited electron dynamics is crucial for light-induced energy transfer.
• Analyzing complex molecular aggregates presents significant computational challenges.

Purpose of the Study:

• Introduce a practical calculation scheme for excited electron dynamics in molecular aggregates.
• Facilitate the analysis of time-dependent excitation and electron migration.
• Incorporate light-electron couplings into the theoretical framework.

Main Methods:

• Developed a local group diabatic Fock representation for excited electron dynamics.
• Implemented a scheme to analyze interacting time-dependent excitation of local sites.
• Considered light-electron couplings within the calculation.

Main Results:

• The scheme simplifies the analysis of excited electron dynamics in complex systems.
• Applied the method to a naphthalene-tetracyanoethylene dimer and a 20-mer ethylene circle.
• Local group analysis provided intuitive understanding of electron transfers between monomers.

Conclusions:

• The presented scheme offers a practical approach for studying electron migration in light-induced energy transfer.
• The method enables intuitive analysis of electron dynamics and transfer pathways.
• Applicable to various molecular aggregate systems for fundamental research.