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Record W1996306546 · doi:10.1063/1.2916714

Universal mathematical identities in density functional theory: Results from three different spin-resolved representations

2008· article· en· W1996306546 on OpenAlexaff
Patricia Pérez, Eduardo Chamorro, Paul W. Ayers

Bibliographic record

VenueThe Journal of Chemical Physics · 2008
Typearticle
Languageen
FieldChemistry
TopicFree Radicals and Antioxidants
Canadian institutionsMcMaster University
Fundersnot available
KeywordsDensity functional theoryRepresentation (politics)Legendre transformationBETA (programming language)Spin (aerodynamics)PhysicsNotationQuantum mechanicsMathematicsComputational chemistryChemistryComputer scienceThermodynamicsArithmetic

Abstract

fetched live from OpenAlex

This paper supersedes previous theoretical approaches to conceptual DFT because it provides a unified and systematic approach to all of the commonly considered formulations of conceptual DFT, and even provides the essential mathematical framework for new formulations. Global, local, and nonlocal chemical reactivity indicators associated with the "closed-system representation" ([N(alpha),N(beta),nu(alpha)(r),nu(beta)(r)]) of spin-polarized density functional theory (SP-DFT) are derived. The links between these indicators and the ones associated with the "open-system representation" ([mu(alpha),mu(beta),nu(alpha)(r),nu(beta)(r)]) are derived, including the spin-resolved Berkowitz-Parr identity. The Legendre transform to the "density representation" ([rho(alpha)(r),rho(beta)(r)]) is performed, and the spin-resolved Harbola-Chattaraj-Cedillo-Parr identities linking the density representation to the closed-system and open-system representations are derived. Taken together, these results provide the framework for understanding chemical reactions from both the electron-following perspective (using either the closed-system or the open-system representation) and electron-preceding perspective (density representation). A powerful matrix-vector notation is developed; with this notation, identities in conceptual DFT become universal. Specifically, this notation allows the fundamental identities in conventional (spin-free) conceptual DFT, the [N(alpha),N(beta)] representation, and the [N=N(alpha)+N(beta),N(S)=N(alpha)-N(beta)] representation to be written in exactly the same forms. In cases where spin transfer and electron transfer are coupled (e.g., radical+molecule reactions), we believe that the [N(alpha),N(beta)] representation may be more useful than the more common [N,N(S)] representation.

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 distilled prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesnone
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.449
Threshold uncertainty score0.366

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0000.000

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 head0.032
GPT teacher head0.242
Teacher spread0.211 · 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 teacher head, not a consensus.

The models applied no category: nothing in the taxonomy fit this work.
Study designBench or experimental
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

Citations81
Published2008
Admission routes1
Has abstractyes

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