Response calculations with an independent particle system with an exact one-particle density matrix

K.J.H. Giesbertz, O.V. Gritsenko, E.J. Baerends

Research output: Contribution to JournalArticleAcademicpeer-review

Abstract

We use the natural orbitals to define an independent particle system, from which the exact one-particle density matrix can be obtained with an ensemble of degenerate determinantal ground states. Also defining explicit phases for the orbitals, and admitting functionals that are dependent on those phases, time-dependent equations for the orbitals and occupation numbers are obtained from an action principle. The wrong polarizability and lack of double excitations of straightforward adiabatic time-dependent density matrix functional theory are then corrected, and the important symmetry χ(ω)=χ
Original languageEnglish
Article number013002
Number of pages4
JournalPhysical Review Letters
Volume105
Issue number1
DOIs
Publication statusPublished - 2010

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