Physics – Condensed Matter – Mesoscale and Nanoscale Physics
Scientific paper
2010-08-09
Physics
Condensed Matter
Mesoscale and Nanoscale Physics
26 pages, 12 figures
Scientific paper
In so far as time-dependent density-functional theory (TDDFT) provides an exact formalism for calculating molecular absorption spectra, TDDFT should be able to describe not only 1- electron excited states but also 2-electron, 3-electron, etc. excited states which show up in molecular spectra by borrowing intensity from 1-electron excited states. This requires going beyond conventional adiabatic TDDFT where the exchange-correlation kernel is frequency in- dependent, fxc, to include an appropriate frequency dependence, fxc(\omega). Maitra, Zhang, Cave, and Burke gave a heuristic derivation of a frequency-dependent correction to adiabatic TDDFT (an approach they called "dressed TDDFT") designed to bring in one double excitation [J. Chem. Phys. 120, 5932 (2004)] and Casida showed how dressed TDDFT might be generalized in the form of a polarization propagator (PP) correction to adiabatic TDDFT [J. Chem. Phys. 122, 054111 (2005)]. This paper presents a further exploration of the PP approach to dressed TDDFT using an approach which is significantly more rigorous than previous dressed TDDFT work and previous work on a PP correction to adiabatic TDDFT. A link is also made with work based directly upon the Bethe-Salpeter equation. At first order we recover the exact exchange result of G\"orling [Int. J. Quant. Chem. 69, 265 (1998).] A second-order treatment brings in 2-electron excitations. An important result of Gonze and Scheffler [Phys. Rev. Lett. 82, 4416 (1999)] emerges as a trivial consequence of this formalism. Concrete formulae for the nonadia- batic correction are derived at the level of the second-order polarization propagator (SOPPA) and algebraic diagrammatic construction (ADC) approaches. The example of butadiene is used to make a connection with the pioneering dressed theory of Maitra et al.
Casida Mark E.
Huix-Rotllant Miquel
No associations
LandOfFree
Formal Foundations of Dressed Time-Dependent Density-Functional Theory for Many-Electron Excitations does not yet have a rating. At this time, there are no reviews or comments for this scientific paper.
If you have personal experience with Formal Foundations of Dressed Time-Dependent Density-Functional Theory for Many-Electron Excitations, we encourage you to share that experience with our LandOfFree.com community. Your opinion is very important and Formal Foundations of Dressed Time-Dependent Density-Functional Theory for Many-Electron Excitations will most certainly appreciate the feedback.
Profile ID: LFWR-SCP-O-83558