English

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

Chemical Physics 2014-03-10 v3 Materials Science Quantum Physics

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 (ω0\omega\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 H2_2 and compare the performance of two different two-electron functionals: the phase-including L\"owdin-Shull functional and the density matrix form of the L\"owdin-Shull functional.

Keywords

Cite

@article{arxiv.1311.3544,
  title  = {Response calculations based on an independent particle system with the exact one-particle density matrix: polarizabilities},
  author = {Klaas J. H. Giesbertz and Oleg V. Gritsenko and Evert Jan Baerends},
  journal= {arXiv preprint arXiv:1311.3544},
  year   = {2014}
}

Comments

10 pages, 6 figures