Response calculations based on an independent particle system with the exact one-particle density matrix: polarizabilities

Abstract

Recently, we have demonstrated that the problems finding a suitable adiabatic approximation in time-dependent one-body reduced density matrix functional theory can be remedied by introducing an additional degree of freedom to describe the system: the phase of the natural orbitals [Phys. Rev. Lett. 105, 013002 (2010), J. Chem. Phys. 133, 174119 (2010)]. In this article we will show in detail how the frequency-dependent response equations give the proper static limit ($\omega \to 0$), including the perturbation in the chemical potential, which is required in static response theory to ensure the correct number of particles. Additionally we show results for the polarizability for H${}_2$ and compare the performance of two different two-electron functionals: the phase-including Löwdin-Shull functional and the density matrix form of the Löwdin-Shull functional.

10 pages, 6 figures

References in corpus (5)

• On the "Causality Paradox" of Time-Dependent Density Functional Theory
• Global fixed point proof of time-dependent density-functional theory
• Adiabatic approximation in time-dependent reduced-density-matrix functional theory
• Time-dependent occupation numbers in reduced-density-matrix functional theory: Application to an interacting Landau-Zener model
• Hamiltonian formulation of nonequilibrium quantum dynamics: geometric structure of the BBGKY hierarchy

Cited by in corpus (4)

• CHEERS: A tool for Correlated Hole-Electron Evolution from Real-time Simulations
• One-body reduced density-matrix functional theory in finite basis sets at elevated temperatures
• Implications of the unitary invariance and symmetry restrictions on the development of proper approximate one-body reduced density matrix functionals
• The dissection algorithm for the second-Born self-energy