Beyond quantum mean-field approximation: Phase-space formulation of many-body time-dependent density functional theory and efficient spectral approximations

Abstract

As a universal quantum mechanical approach to the dynamical many-body problem, the time-dependent density functional theory (TDDFT) might be inadequate to describe crucial observables that rely on two-body evolution behavior, like the double-excitation probability and two-body dynamic correlation. One promising remedy is to utilize the time-dependent 2-reduced density matrix (2-RDM) that directly represents two-body observables in an N-particle system, and resort to the extended TDDFT for multibody densities to break the confines of spatial local on one-body density [Phys. Rev. Lett. 26(6) (2024) 263001]. However, the usage of 2-RDM is prohibitive due to the augmented dimensionality, e.g., 4-D space for unidimensional 2-RDM. This work addresses the high-dimensional numerical challenges by using an equivalent Wigner phase-space formulation of 2-RDM and seeking efficient spectral approximations to nonlocal quantum potentials. For spatial periodic case, a pseudo-difference operator approach is derived for both the Hartree-exchange-correlation term and two-body collision operator, while the discretization via the Chebyshev spectral element method is provided for non-periodic case. A massively parallel numerical scheme, which integrates these spectral approximations with a distributed characteristics method, allows us to make the first attempt for real simulations of 2-RDM dynamics. Numerical experiments demonstrate the two-body correction to the quantum kinetic theory, and show the increase in the system's entropy induced by the two-bdoy interaction. Thus it may pave the way for an accurate description of 2-RDM dynamics and advance to a practical application of many-body TDDFT.