Analyzing Excitation-Energy Transfer Based on the Time-Dependent Density Functional Theory in Real Time

Area of Science:

• Quantum chemistry
• Computational physics
• Photochemistry

Background:

• Excitation-energy transfer is crucial for light-energy conversion processes like photosynthesis.
• Accurate simulation of these processes is computationally demanding.

Purpose of the Study:

• To demonstrate the application of real-time time-dependent density functional theory (DFT) for analyzing excitation-energy transfer.
• To introduce novel measures of energy transfer grounded in DFT.

Main Methods:

• Utilizing real-time time-dependent DFT for first-principles simulations.
• Developing measures of energy transfer based on time-dependent electron density.
• Applying methods to model systems with static and dynamic nuclei (DFT-based Ehrenfest dynamics).

Main Results:

• Demonstrated the feasibility of simulating excitation-energy transfer using real-time DFT.
• Introduced DFT-based measures that are intuitive and reproduce analytical model limits.
• Validated the approach for both static and dynamic nuclear scenarios.

Conclusions:

• Real-time DFT provides an efficient and accurate framework for studying excitation-energy transfer.
• The developed density-based measures offer valuable insights into energy transfer mechanisms.
• This approach is applicable to complex systems in photochemistry and beyond.