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Record W2049237853 · doi:10.1002/qua.10607

Potential energy barriers for dissociative attachment to HF.HF and HCl.HCl: Ab initio study

2003· article· en· W2049237853 on OpenAlexafffund
Arvi Rauk, David A. Armstrong

Bibliographic record

VenueInternational Journal of Quantum Chemistry · 2003
Typearticle
Languageen
FieldPhysics and Astronomy
TopicAdvanced Chemical Physics Studies
Canadian institutionsUniversity of Calgary
FundersNatural Sciences and Engineering Research Council of CanadaUniversity of Calgary
KeywordsChemistryDimerAb initioValence (chemistry)Endothermic processDipoleIonTransition stateComputational chemistryPhysical chemistryCatalysis

Abstract

fetched live from OpenAlex

Abstract Dissociative attachment (DA) of an electron to the dimers of HF and HCl, reaction (1) equation image has been investigated by theoretical calculations at MP2 and CCSD(T) levels with large basis sets. Transition structures (TSs) for the loss of an H atom and formation of the FHF − and ClHCl − anions were located by analytic methods. Initial electron attachment to HF.HF dimer occurs without activation and yields a dipole‐bound anion state (DBS) as shown previously. Reaction (1) is endothermic by 65.8 kJ/mol at the CCSD(T)/aug‐cc‐pVDZ level. An intermediate ion‐induced dipole complex between H · and FHF − is reached from the DBS over a potential barrier of 66.6 kJ/mol. Analysis of the charge distribution as a function of the distance to the departing H · reveals that the diffuse DBS collapses to a much more compact valence configuration prior to the TS being reached. In the valence configuration, the electron occupies the σ* orbital of the terminal HF bond. DA to HCl.HCl differs from the fluorine case in several important respects. HCl.HCl does not form a DBS. Rather, electron attachment occurs by direct insertion into the σ* orbital of the terminal HCl bond with an activation energy of 20.3 kJ/mol. As in the fluorine case, electron capture occurs before the TS. The electron density collapses to a valence configuration when the HCl bond is stretched to about 1.45 Å, intermediate between that in the neutral dimer, 1.28 Å, and in the TS to DA, 1.57 Å. A “T‐shaped” ion‐induced dipole complex, bound by about 2 kJ/mol, lies between the TS and the separated H atom and ClHCl − anion products. With respect to DA, the chlorine system is intermediate between the fluorine system and the previously reported bromine system. The latter was found to undergo DA with a 0.0‐kJ/mol barrier. © 2003 Wiley Periodicals, Inc. Int J Quantum Chem, 2003

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 score0.226
Threshold uncertainty score0.617

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 head0.009
GPT teacher head0.301
Teacher spread0.292 · 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

Citations7
Published2003
Admission routes2
Has abstractyes

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