An investigation of hybridization and the orbital models of molecular electronic structure for CH<sub>4</sub>, NH<sub>3</sub>, and H<sub>2</sub>O
Bibliographic record
Abstract
Observations of the physical behaviour (motions) of the valence (frontier) electrons in the iconic benchmark hydride molecules CH 4 , NH 3 , and H 2 O are used to provide a direct experimental evaluation of hybridization and of the localized and delocalized orbital models of molecular electronic structure, after more than 80 years since the initial proposals of these theoretical concepts. Our previously published experimental measurements of valence (frontier) electron momentum probability distributions, made by electron momentum spectroscopy (EMS), are compared with those calculated using the localized molecular orbital (LMO) model and a range of hybrid orbital models, as well as with the delocalized canonical molecular orbital (CMO) and density functional theory Kohn–Sham orbital (KSO) models. In all cases, the electron momentum probability distributions calculated with LMOs and localized hybrid orbital type models are inconsistent with the experimental observations. In contrast, those calculated with the delocalized CMOs and KSOs are in very good agreement with the experimental measurements. These findings are of importance in those research applications such as reactivity, drug and novel material design, and also in molecular electronics, where the shapes and orientations of particular valence (frontier) orbital electron density probability distributions (and not the total electron densities) are considered to be key determining factors. These findings and their implications are also of pedagogical significance in chemistry and molecular physics.
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot 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.
Distilled classifier scores by category (both heads)
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.001 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.001 |
| Scholarly communication | 0.000 | 0.001 |
| Open science | 0.000 | 0.001 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.002 | 0.000 |
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.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.
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".