Calculation of screened Coulomb interaction parameters for the charge-disproportionated insulator CaFeO$_3$

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Main Authors: Merkel, Maximilian E., Ederer, Claude
Format: Preprint
Published: 2023
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author Merkel, Maximilian E.
Ederer, Claude
author_facet Merkel, Maximilian E.
Ederer, Claude
contents We calculate the screened electron-electron interaction for the charge-disproportionated insulator CaFeO$_3$ using the constrained random-phase approximation (cRPA). While in many correlated materials, the formation of a Mott-insulating state is driven by a large local Coulomb repulsion, represented by the Hubbard $U$, several cases have been identified more recently where $U$ is strongly screened and instead the Hund's interaction $J$ dominates the physics. Our results confirm a strong screening of the local Coulomb repulsion $U$ in CaFeO$_3$ whereas $J$ is much less screened and can thus stabilize a charge-disproportionated insulating state. This is consistent with the case of the rare-earth nickelates where similar behavior has been demonstrated. In addition, we validate some common assumptions used for parametrizing the local electron-electron interaction in first-principles calculations based on density-functional theory (DFT), assess the dependence of the interaction on the choice of correlated orbitals, and discuss the use of the calculated interaction parameters in DFT+$U$ calculations of CaFeO$_3$. Our work also highlights certain limitations for the direct use of cRPA results in DFT-based first-principles calculations, in particular for systems with strong entanglement between the correlated and uncorrelated bands.
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institution arXiv
publishDate 2023
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spellingShingle Calculation of screened Coulomb interaction parameters for the charge-disproportionated insulator CaFeO$_3$
Merkel, Maximilian E.
Ederer, Claude
Strongly Correlated Electrons
Computational Physics
We calculate the screened electron-electron interaction for the charge-disproportionated insulator CaFeO$_3$ using the constrained random-phase approximation (cRPA). While in many correlated materials, the formation of a Mott-insulating state is driven by a large local Coulomb repulsion, represented by the Hubbard $U$, several cases have been identified more recently where $U$ is strongly screened and instead the Hund's interaction $J$ dominates the physics. Our results confirm a strong screening of the local Coulomb repulsion $U$ in CaFeO$_3$ whereas $J$ is much less screened and can thus stabilize a charge-disproportionated insulating state. This is consistent with the case of the rare-earth nickelates where similar behavior has been demonstrated. In addition, we validate some common assumptions used for parametrizing the local electron-electron interaction in first-principles calculations based on density-functional theory (DFT), assess the dependence of the interaction on the choice of correlated orbitals, and discuss the use of the calculated interaction parameters in DFT+$U$ calculations of CaFeO$_3$. Our work also highlights certain limitations for the direct use of cRPA results in DFT-based first-principles calculations, in particular for systems with strong entanglement between the correlated and uncorrelated bands.
title Calculation of screened Coulomb interaction parameters for the charge-disproportionated insulator CaFeO$_3$
topic Strongly Correlated Electrons
Computational Physics
url https://arxiv.org/abs/2310.16541