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Record W1991803932 · doi:10.1021/jp902792n

Chemical Reactivity Descriptors for Ambiphilic Reagents: Dual Descriptor, Local Hypersoftness, and Electrostatic Potential

2009· article· en· W1991803932 on OpenAlex

Why this work is in the frame

A frame that forgets how it found something cannot be audited. These are the routes that admitted this work.

affAt least one author lists a Canadian institution in the pinned OpenAlex snapshot.

Bibliographic record

VenueThe Journal of Physical Chemistry A · 2009
Typearticle
Languageen
FieldChemistry
TopicOrganic Chemistry Cycloaddition Reactions
Canadian institutionsMcMaster University
Fundersnot available
KeywordsNucleophileChemistryElectrophileReactivity (psychology)ReagentMoleculeComputational chemistryDual (grammatical number)Combinatorial chemistryElectronElectron acceptorElectron transferChemical physicsPhotochemistryOrganic chemistryPhysicsCatalysisQuantum mechanics

Abstract

fetched live from OpenAlex

The second-order response of the electron density with respect to changes in electron number, known as the dual descriptor, has been established as a key reactivity indicator for reactions like pericyclic reactions, where reagents accept and donate electrons concurrently. Here we establish that the dual descriptor is also the key reactivity indicator for ambiphilic reagents: reagents that can act either as electrophiles or as nucleophiles, depending on the reaction partner. Specifically, we study dual atoms (which are proposed to act, simultaneously, as an electron acceptor and an electron donor), dual molecules (which react with both electrophiles and nucleophiles, generally at different sites), and dual ion-molecule complexes (which react with both cations and anions). On the basis of our analysis, the dual atom (an Al(I) that has been purported to be dual in the literature) is actually pseudodual in the sense that it does not truly accept electrons from a nucleophiles; rather, it serves as a conduit through which an electrophile can donate electrons to the attached aromatic ring. For understanding dual ion-molecule complexes, it helps to understand that the dual descriptor makes a key contribution to the long-range portion of the quadratic hyperpolarization. In all cases, a complete description of the reactivity of the ambiphilic reagent requires considering both an orbital-based descriptor of electron transfer (the dual descriptor or the local hypersoftness) and the electrostatic potential. The local hypersoftness strongly resembles the dual descriptor.

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.

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 categoriesMeta-epidemiology (narrow)
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 score0.002
Threshold uncertainty score1.000

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 integrity0.0000.001
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 head0.007
GPT teacher head0.222
Teacher spread0.215 · 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