Adiabatic approximation within time-dependent density functional theory using inversion of the ground-state spin-density Kohn–Sham formalism

Dreissigacker, Ingo; Lein, Manfred

doi:10.1016/j.chemphys.2011.02.009

Cited by 7 publications

(4 citation statements)

References 24 publications

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“…We also increase the update to the potential in regions of low density by simply using the inverse of the density (up to a maximum value) as a weighting factor, as in Ref. [30]. When the density converges to the target density, we have found v adia all potential of Eq.…”

Section: B the Exact Adiabatic Approximationmentioning

confidence: 99%

“…This state is not a spin-eigenstate (although it does have S = 0), but is a valid choice for an initial KS state, having the same total density as the true system. The up and down spin-densities are not equal, and we shall evolve them in different spin-up and spin-down KS potentials, but, unlike in spin-DFT, we do not consider the spin-densities separately meaningful; only their sum is considered as an observable [30]. Instead, (c) will be used to illustrate the effects of orbital-specific functionals, as will be discussed more later.…”

Section: Initial-state Dependence In Tddftmentioning

confidence: 99%

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Propagation of initially excited states in time-dependent density-functional theory

Elliott

Maitra

2012

Phys. Rev. A

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Many recent applications of time-dependent density functional theory begin in an initially excited state and propagate it using an adiabatic approximation for the exchange-correlation potential. This, however, inserts the excited-state density into a ground-state approximation.By studying a series of model calculations, we highlight the relevance of initial-state dependence of the exact functional when starting in an excited state, discuss different valid choices of the initial Kohn-Sham state, and explore the errors inherent in the adiabatic approximation that neglects this dependence.

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Section: B the Exact Adiabatic Approximationmentioning

confidence: 99%

Section: Initial-state Dependence In Tddftmentioning

confidence: 99%

Propagation of initially excited states in time-dependent density-functional theory

Elliott

Maitra

2012

Phys. Rev. A

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“…We further demonstrate the mechanism through which a local potential can lead to neutral dissociation and present a detailed analysis of its "step structure" features. The study gains further significance as the physics of this "step structure" in the exchange-correlation potential, which is at the heart of the dissociation problem, is also highly relevant to problems of ionization by external fields [33,34].…”

Section: Introductionmentioning

confidence: 99%

Dissociation of diatomic molecules and the exact-exchange Kohn-Sham potential: The case of LiF

2011

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We examine the role of the exact-exchange (EXX) Kohn-Sham potential in curing the problem of fractional molecular dissociation. This is achieved by performing EXX calculations for the illustrative case of the LiF molecule. We show that by choosing the lowest-energy electronic configuration for each interatomic distance, a qualitatively correct binding energy curve, reflecting integer dissociation, is obtained. Surprisingly, for LiF this comes at the cost of violating the Aufbau principle, a phenomenon we discuss at length. Furthermore, we numerically confirm that in the EXX potential of the diatomic molecule, one of the atomic potentials is shifted by a constant while the other one is not, depending on where the highest occupied molecular orbital is localized. This changes the relative positions of the energies of each atom and enforces the integer configuration by preventing spurious charge transfer. The size of the constant shift becomes increasingly unstable numerically the larger the interatomic separation is, reflecting the increasing absence of coupling between the atoms.

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“…In [32] it was shown that the results can be improved by including a quasidiscontinuous behavior by hand, leading to a knee structure in the double ionization yield and to an increased single-ionization yield. Systematic approaches to construct approximations respecting the discontinuity have been proposed, but have not yet found wide-spread application in strong-field ionization [34][35][36]. It should be noted that the calculation of the single-and doubleionization yields from the density is a further issue in TDDFT, which we do not address in depth in the present paper.…”

Section: Introductionmentioning

confidence: 91%

Time-dependent density functional theory for strong-field ionization by circularly polarized pulses

Chirilă

Lein

2017

J. Phys. B: At. Mol. Opt. Phys.

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By applying time-dependent density functional theory to a two-dimensional multielectron atom subject to strong circularly polarized light pulses, we confirm that the ionization of p orbitals with defined angular momentum depends on the sense of rotation of the applied field. A simple ad-hoc modification of the adiabatic local-density exchange-correlation functional is proposed to remedy its unphysical behavior under orbital depletion.

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Adiabatic approximation within time-dependent density functional theory using inversion of the ground-state spin-density Kohn–Sham formalism

Cited by 7 publications

References 24 publications

Propagation of initially excited states in time-dependent density-functional theory

Propagation of initially excited states in time-dependent density-functional theory

Dissociation of diatomic molecules and the exact-exchange Kohn-Sham potential: The case of LiF

Time-dependent density functional theory for strong-field ionization by circularly polarized pulses

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