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

Excitation-energy transfer is a key step in processes such as photosynthesis that convert light into other forms of energy. Time-dependent density functional theory (DFT) in real time is ideal for the first-principles simulation of such processes due to its computational efficiency. We here demonstrate how real-time DFT can be used for analyzing excitation-energy transfer from first-principles. We discuss several measures of energy transfer that are based solely on the time-dependent density, are well founded in the DFT framework, allow for intuitive understanding and visualization, and reproduce important limiting cases of an analytical model. We demonstrate their usefulness in calculations for model systems, both with static nuclei and in the context of DFT-based Ehrenfest dynamics.