Propagating two-particle reduced density matrices without wavefunctions

TL;DR

This paper introduces a novel time-dependent many-body theory based on the two-particle reduced density matrix, enabling stable and accurate simulations of correlated electron dynamics in systems with strong interactions.

Contribution

It develops a closed equation of motion for the 2-RDM with a new reconstruction functional that maintains key physical symmetries and $N$-representability during time evolution.

Findings

Accurately reproduces exact solutions for a 1D LiH model in strong laser fields.

Maintains norm, energy, and spin symmetries during time propagation.

Enables stable simulation of long-range Coulomb interactions in many-body systems.

Abstract

Describing time-dependent many-body systems where correlation effects play an important role remains a major theoretical challenge. In this paper we develop a time-dependent many-body theory that is based on the two-particle reduced density matrix (2-RDM). We develop a closed equation of motion for the 2-RDM employing a novel reconstruction functional for the three-particle reduced density matrix (3-RDM) that preserves norm, energy, and spin symmetries during time propagation. We show that approximately enforcing $N$-representability during time evolution is essential for achieving stable solutions. As a prototypical test case which features long-range Coulomb interactions we employ the one-dimensional model for lithium hydride (LiH) in strong infrared laser fields. We probe both one-particle observables such as the time-dependent dipole moment and two-particle observables such as the pair density and mean electron-electron interaction energy. Our results are in very good agreement with numerically exact solutions for the $N$-electron wavefunction obtained from the multiconfigurational time-dependent Hartree-Fock method.