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arXiv · 1311.3544

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

Klaas J. H. Giesbertz·Oleg V. Gritsenko·Evert Jan Baerends
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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 ($ω\to0$), 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.

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Klaas J. H. Giesbertz, Oleg V. Gritsenko, Evert Jan Baerends. 2014-03-07. Response calculations based on an independent particle system with the exact one-particle density matrix: polarizabilities. https://doi.org/10.1063/1.4867000

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