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Record W2010983131 · doi:10.1103/physrevb.76.155123

<i>Ab initio</i>evaluation of Coulomb and exchange parameters for<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:mi>DFT</mml:mi><mml:mo>+</mml:mo><mml:mi mathvariant="normal">U</mml:mi></mml:mrow></mml:math>calculations

2007· article· lv· W2010983131 on OpenAlexfundno aff
Nicholas J. Mosey, Emily A. Carter

Bibliographic record

VenuePhysical Review B · 2007
Typearticle
Languagelv
FieldPhysics and Astronomy
TopicAdvanced Chemical Physics Studies
Canadian institutionsnot available
FundersArmy Research OfficeNatural Sciences and Engineering Research Council of Canada
KeywordsAb initioCoulombDensity functional theoryPhysicsAtomic orbitalAb initio quantum chemistry methodsAtomic physicsElectronQuantum mechanicsMolecule

Abstract

fetched live from OpenAlex

Conventional density functional theory (DFT) fails for materials with strongly correlated electrons, such as late transition metal oxides. Large errors in the intra-atomic Coulomb and exchange interactions are the source of this failure. The $\mathrm{DFT}+\mathrm{U}$ method has provided a means, through empirical parameters, to correct these errors. Here, we present a systematic ab initio approach in evaluating the intra-atomic Coulomb and exchange terms, $U$ and $J$, respectively, in order to make the $\mathrm{DFT}+\mathrm{U}$ method a fully first-principles technique. The method is based on a relationship between these terms and the Coulomb and exchange integrals evaluated in the basis of unrestricted Hartree-Fock molecular orbitals that represent localized states of the extended system. We used this ab initio scheme to evaluate $U$ and $J$ for chromia $({\mathrm{Cr}}_{2}{\mathrm{O}}_{3})$. The resulting values are somewhat higher than those determined earlier either empirically or in constrained DFT calculations but have the advantage of originating from an ab initio theory containing exact exchange. Subsequent $\mathrm{DFT}+\mathrm{U}$ calculations on chromia using the ab initio derived $U$ and $J$ yield properties consistent with experiment, unlike conventional DFT. Overall, the technique developed and tested in this work holds promise in enabling accurate and fully predictive $\mathrm{DFT}+\mathrm{U}$ calculations of strongly correlated electron materials.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

How this classification was reachedexpand

Full frame machine prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.

metaresearch head score (Codex)0.001
metaresearch head score (Gemma)0.002
Version: metacan-v3-hybrid-931329e0061cValidation status: machine_predicted_unvalidated
Candidate categoriesnone
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Simulation or modeling · Consensus signal: Simulation or modeling
GenreCandidate signal: Empirical · Consensus signal: none
Teacher disagreement score0.009
Threshold uncertainty score0.021

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0010.002
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0010.001
Science and technology studies0.0020.000
Scholarly communication0.0010.001
Open science0.0010.000
Research integrity0.0010.001
Insufficient payload (model declined to judge)0.0060.001

Machine scores (provisional)

The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.

Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.

Opus teacher head0.031
GPT teacher head0.294
Teacher spread0.263 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it

Classification

machine, unvalidated

Machine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.

The models applied no category: nothing in the taxonomy fit this work.
Study designSimulation or modeling
Domainnot available
GenreEmpirical

How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".

Quick stats

Citations242
Published2007
Admission routes1
Has abstractyes

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Same venuePhysical Review BSame topicAdvanced Chemical Physics StudiesFrench-language works237,207