Extended Time-Dependent Density Functional Theory for Multi-Body Densities

Abstract

Time-dependent density functional theory (TDDFT) is widely used for understanding and predicting properties and behaviors of matter. As one of the fundamental theorems in TDDFT, van Leeuwen's theorem [Phys. Rev. Lett. 82, 3863 (1999)] guarantees how to construct a unique potential with the same one-body density evolution. Here we extend van Leeuwen's theorem by exploring truncation criteria in BBGKY-hierarchy. Our generalized theorem demonstrates the existence of a unique non-local potential to accurately reconstruct the multi-body density evolution in binary interacting systems. Under non-stringent conditions, truncation of the BBGKY-hierarchy equations aligns with the behavior of multi-body density evolution, and maintains consistency in the reduced equations. As one of applications within the extended TDDFT supported by our theorem, multiple excitation energy can be typically solved as the eigenvalue of a generalized Casida's equation. The extended TDDFT provides an accurate and first-principle framework capable of describing the kinetic processes of correlated system, including strongly coupled particle transport, multiple excitation and ionization processes.