Self-consistency in frozen-density embedding theory based calculations

Aquilante, Francesco; Wesołowski, Tomasz Adam

doi:10.1063/1.3624888

Cited by 23 publications

(24 citation statements)

References 51 publications

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“…In other cases, omitting this term completely (in the energy functional and in the embedding potential) does not invalidate the key feature of FDET: the energy evaluated with this potential will still be the upper bound of the groundstate energy of the total system. Numerical examples show 29 even if the simplest form (single determinant) of the embedded wavefunction. Until now, we kept the F MD [ρ A ] term in all equations for the sake of completeness and generality-to include methods which do not take into account the correlation effects within the embedded subsystem completely.…”

Section: Fdet and Beyond-fdet Approximate Methods For Excited Stmentioning

confidence: 99%

Embedding potentials for excited states of embedded species

Wesołowski

2014

The Journal of Chemical Physics

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Frozen-Density-Embedding Theory (FDET) is a formalism to obtain the upper bound of the groundstate energy of the total system and the corresponding embedded wavefunction by means of EulerLagrange equations [T. A. Wesolowski, Phys. Rev. A 77(1), 012504 (2008)]. FDET provides the expression for the embedding potential as a functional of the electron density of the embedded species, electron density of the environment, and the field generated by other charges in the environment. Under certain conditions, FDET leads to the exact ground-state energy and density of the whole system. Following Perdew-Levy theorem on stationary states of the ground-state energy functional, the other-than-ground-state stationary states of the FDET energy functional correspond to excited states. In the present work, we analyze such use of other-than-ground-state embedded wavefunctions obtained in practical calculations, i.e., when the FDET embedding potential is approximated. Three computational approaches based on FDET, that assure self-consistent excitation energy and embedded wavefunction dealing with the issue of orthogonality of embedded wavefunctions for different states in a different manner, are proposed and discussed.

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Section: Fdet and Beyond-fdet Approximate Methods For Excited Stmentioning

confidence: 99%

Embedding potentials for excited states of embedded species

Wesołowski

2014

The Journal of Chemical Physics

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“…Examples include Amsterdam Density-Functional (ADF) [101], TURBOMOLE [99,102], deMon [36,103], Dirac [104], Q-Chem [45], and MolCas [105]. The number of features and the flexibility of the implementations may vary, but all of them share some important similarities, such as the use of localized atom-centered basis sets (Slater or Gaussian type).…”

Section: Applications Of Subsystem Dft 221 Molecular Systems: Localmentioning

confidence: 99%

Subsystem density-functional theory as an effective tool for modeling ground and excited states, their dynamics and many-body interactions

Krishtal

Sinha

Genova

et al. 2015

J. Phys.: Condens. Matter

113

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Subsystem Density-Functional Theory (DFT) is an emerging technique for calculating the electronic structure of complex molecular and condensed phase systems. In this topical review, we focus on some recent advances in this field related to the computation of condensed phase systems, their excited states, and the evaluation of many-body interactions between the subsystems. As subsystem DFT is in principle an exact theory, any advance in this field can have a dual role. One is the possible applicability of a resulting method in practical calculations. The other is the possibility of shedding light on some quantummechanical phenomenon which is more easily treated by subdividing a supersystem into subsystems. An example of the latter is many-body interactions. In the discussion, we present some recent work from our research group as well as some new results, casting them in the current state-of-the-art in this review as comprehensively as possible.2

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“…The full embedding kernel contribution can be expressed as (63) with the delta function indicating that the Coulomb term is only evaluated for the inter-subsystem interaction (i = j). For convenience, we introduce auxiliary kernel contributions to specify the kinetic energy and exchange-correlation terms in the embedding kernel,…”

Section: B Dft-in-dft Response Theorymentioning

confidence: 99%

Molecular properties via a subsystem density functional theory formulation: A common framework for electronic embedding

Höfener¹,

Gomes

Visscher³

2012

The Journal of Chemical Physics

107

125

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In this article, we present a consistent derivation of a density functional theory (DFT) based embedding method which encompasses wave-function theory-in-DFT (WFT-in-DFT) and the DFT-based subsystem formulation of response theory (DFT-in-DFT) by Neugebauer [J. Neugebauer, J. Chem. Phys. 131, 084104 (2009)] as special cases. This formulation, which is based on the time-averaged quasi-energy formalism, makes use of the variation Lagrangian techniques to allow the use of nonvariational (in particular: coupled cluster) wave-function-based methods. We show how, in the timeindependent limit, we naturally obtain expressions for the ground-state DFT-in-DFT and WFT-in-DFT embedding via a local potential. We furthermore provide working equations for the special case in which coupled cluster theory is used to obtain the density and excitation energies of the active subsystem. A sample application is given to demonstrate the method.

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Self-consistency in frozen-density embedding theory based calculations

Cited by 23 publications

References 51 publications

Embedding potentials for excited states of embedded species

Embedding potentials for excited states of embedded species

Subsystem density-functional theory as an effective tool for modeling ground and excited states, their dynamics and many-body interactions

Molecular properties via a subsystem density functional theory formulation: A common framework for electronic embedding

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