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Record W1983328144 · doi:10.1021/jp102822c

On the Formation of Proton-Shared and Contact Ion Pair Forms during the Dissociation of Moderately Strong Acids: An Ab Initio Molecular Dynamics Investigation

2010· article· en· W1983328144 on OpenAlexaff
Vibin Ipe Thomas, Patrick Maurer, Radu Iftimie

Bibliographic record

VenueThe Journal of Physical Chemistry B · 2010
Typearticle
Languageen
FieldPhysics and Astronomy
TopicSpectroscopy and Quantum Chemical Studies
Canadian institutionsUniversité de Montréal
Fundersnot available
KeywordsDissociation (chemistry)IonAb initioMolecular dynamicsProtonChemistryChemical physicsComputational chemistryPhotochemistryPhysical chemistryPhysicsOrganic chemistryNuclear physics

Abstract

fetched live from OpenAlex

Acid ionization and dissociation are phenomena that play a fundamental role in chemistry and biology, but their microscopic details are largely unknown. We use ab initio molecular dynamics to identify and characterize various structures that are formed along the pathway of dissociation of trifluoroacetic acid (p K a = 0.5). The present results demonstrate that solutions of moderately strong (−1 ≤ p K a ≤ 1) carboxylic acids contain significant quantities of at least two forms whose bonding patterns are intermediate between those of covalent and dissociated structures, R−COOH···OH 2 and R−COO − (aq) + H 3 O + (aq), respectively. The first is a proton-shared structure of the form R−COO δ− ·H· δ+ OH 2 which can be distinguished from the covalent form by its characteristic “continuous” absorption below 1700 cm −1 . The second is a contact ion pair whose average structure can be written as R−COO − ·H 3 O + . We demonstrate that the transformation of proton-shared into contact ion pair forms coincides with the disappearance of the carbonyl vibration mode centered around 1720 cm −1 and the appearance of the asymmetric and symmetric carboxylate vibration modes at 1620 and 1380 cm −1, respectively. The aforementioned transformation is accompanied by significant changes in the first solvation shell of the acid molecule which we discuss.

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 machine prediction

Teacher imitation

Not 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.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: metacan-v3-hybrid-931329e0061cValidation status: machine_predicted_unvalidated
Candidate categoriesnone
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Simulation or modeling · Consensus signal: Simulation or modeling
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.003
Threshold uncertainty score0.006

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0010.001
Scholarly communication0.0000.001
Open science0.0010.000
Research integrity0.0010.000
Insufficient payload (model declined to judge)0.0010.000

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 head0.008
GPT teacher head0.240
Teacher spread0.231 · 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 source (direct Gemma or distilled Codex), not a consensus.

The models applied no category: nothing in the taxonomy fit this work.
Study designSimulation or modeling
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

Citations13
Published2010
Admission routes1
Has abstractyes

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Same venueThe Journal of Physical Chemistry BSame topicSpectroscopy and Quantum Chemical StudiesFrench-language works237,207