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Record W2060705021 · doi:10.1021/jp911405e

Theoretical Analysis of the Resonance Assisted Hydrogen Bond Based on the Combined Extended Transition State Method and Natural Orbitals for Chemical Valence Scheme<sup>†</sup>

2010· article· en· W2060705021 on OpenAlex
Rafał Kurczab, Mariusz P. Mitoraj, Artur Michalak, Tom Ziegler

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 · 2010
Typearticle
Languageen
FieldChemistry
TopicCrystallography and molecular interactions
Canadian institutionsUniversity of Calgary
Fundersnot available
KeywordsHydrogen bondChemistryValence (chemistry)Chemical bondAtomic orbitalValence bond theoryComputational chemistryHydrogenCovalent bondThree-center two-electron bondLow-barrier hydrogen bondCrystallographyAtomic physicsMolecular orbitalMoleculePhysicsQuantum mechanicsOrganic chemistry

Abstract

fetched live from OpenAlex

We have analyzed hydrogen bonding in a number of species, containing from two to four hydrogen bonds. The examples were chosen in such a way that they would enable us to examine three different hydrogen bonds involving OH-O, NH-O, and NH-N. A common feature of the investigated systems is that they all are expected to exhibit resonance assisted hydrogen bonding (RAHB) in the electronic pi-framework. Our analysis was based on a recently developed method that combines the extended transition state scheme with the theory of natural orbitals for chemical valence (ETS-NOCV). We find that hydrogen bonding is associated with charge rearrangement in both the electronic sigma-framework (Deltarho(sigma)) and the electronic pi-framework (Deltarho(pi)). However the stabilization due to Deltarho(sigma) is four times as important as the stabilization (RAHB) due to Deltarho(pi). Stabilization due to the electrostatic interaction (DeltaE(elstat)) between the two monomers that are brought together to form the hydrogen bonds is also important. However DeltaE(el) cannot alone account for the strength of the hydrogen bonds as it is more than compensated for by the repulsive Pauli repulsion (DeltaE(Pauli)). When N' is part of an aromatic ring, N'H-O and N'H-N bonds are similar in strength to OH-O links involving carboxylic groups. However, NH-O bonds involving amide groups (-NH(2)) are considerably weaker than the OH-O links mentioned above. In systems with different hydrogen bonds, their relative strength is determined collectively in such a way as to optimize the total interaction. This can result in that one of the bonds (OH-O, NH-O, and NH-N) becomes particularly strong or exceptionally weak. Even within the same dimer two X'-HX bonds of the same type can show quite different strength.

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)0.001
metaresearch head score (Gemma)0.001
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 score0.175
Threshold uncertainty score0.416

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.001
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.001
Bibliometrics0.0000.000
Science and technology studies0.0000.001
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 head0.006
GPT teacher head0.261
Teacher spread0.255 · 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