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Record W1989007435 · doi:10.1021/jp012642u

An Atoms in Molecules and Electron Localization Function Computational Study on the Molecular Structure of the 6-Tricyclo[3.2.1.0<sup>2,4</sup>]octyl Cation

2001· article· en· W1989007435 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 · 2001
Typearticle
Languageen
FieldChemistry
TopicOrganic Chemistry Cycloaddition Reactions
Canadian institutionsMcMaster University
Fundersnot available
KeywordsDelocalized electronChemistryElectron localization functionMoleculeBond lengthRange (aeronautics)CrystallographyElectronFunction (biology)Single bondComputational chemistryGroup (periodic table)PhysicsMaterials scienceQuantum mechanicsOrganic chemistry

Abstract

fetched live from OpenAlex

The structure of 6-tricyclo[3.2.1.0 2,4 ]octyl cation 1 was optimized at HF, Becke3PW91, Becke3LYP, MP2, and MP2(full) levels with the 6-311G(d,p) basis set. Becke3PW91 and MP2(full) yielded similar values for the geometrical parameters of optimized 1 . When the C4−C6 distance was changed incrementally through the range 1.40−2.32 Å at the Becke3PW91/6-311G(d,p) level, there was no discontinuity in the total energy and the geometrical parameters of the cyclopropyl group underwent marked changes. AIM (the theory of atoms in molecules) and ELF (electron localization function) analyses were carried out to investigate the molecular structure of 1 . No bond path was found between C4 and C6 so 1 is a classical cation without pentacoordinated carbon atoms. Only when the C4−C6 distance was fixed in the range of 1.50−1.62 Å does 1 become a pentacoordinate (nonclassical) species in which C4 is connected to C2, C3, C5, C6, and H13 with bond paths. On the other hand, when the 6-tricyclo[3.2.1.0 2,4 ]octyl cation was substituted with Li and BeH groups at C4 and C5, the optimized equilibrium species exhibted pentacoordinate carbons at C4. Compared with the C1−C2 bond that we take as a normal single bond, the bonds between C4 and C2, C3, C5 are weak, as evidenced by reduced densities ρ ( r ), significantly smaller ∇ 2 ρ ( r ) values, and large ellipticities at the bond critical points (BCPs). The delocalization indices (DIs) the first application of a DI analysis in the study of carbocations for these C−C bonds ranged between 0.733 and 0.860, smaller than unity. The DI between C4 and C6 is 0.634, suggesting that there is a significant degree of homoconjugation between C4 and C6. For polycyclic species such as 1, it appears that a delocalization index of approximately 0.7 and an internuclear distance of 1.6 Å are required for a bond path to materialize between remote carbons. In an ELF analysis we found a small disynaptic basin V(C4,C6) between C4 and C6 that correlated with the existence of a (3, −1) critical point in −∇ 2 ρ ( r ). The properties of ELF disynaptic basins around C4 and a contribution analysis showed a high degree of delocalization at this center.

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 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 score0.108
Threshold uncertainty score0.447

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 head0.004
GPT teacher head0.233
Teacher spread0.228 · 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