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Record W2619945141 · doi:10.1021/jacs.7b01783

Dynamic Disorder and Electronic Structures of Electron-Precise Dianionic Diboranes: Insights from Solid-State Multinuclear Magnetic Resonance Spectroscopy

2017· article· en· W2619945141 on OpenAlexafffund
Y. T. Angel Wong, Johannes Landmann, Maik Finze, David L. Bryce

Bibliographic record

VenueJournal of the American Chemical Society · 2017
Typearticle
Languageen
FieldChemistry
TopicAdvanced NMR Techniques and Applications
Canadian institutionsUniversity of Ottawa
FundersNatural Sciences and Engineering Research Council of CanadaMerck KGaA
KeywordsChemistryCoupling constantResonance (particle physics)CrystallographySpectroscopyBoronMolecular orbitalNuclear magnetic resonance spectroscopyAtomic orbitalSolid-state nuclear magnetic resonanceElectronCoupling (piping)Nuclear magnetic resonanceMolecular physicsMoleculeAtomic physicsStereochemistryPhysics

Abstract

fetched live from OpenAlex

High Resolution Image Download MS PowerPoint Slide The J ( 11 B, 11 B) coupling constants of various salts of the electron-precise hexacyanodiborane(6) dianion, [B 2 (CN) 6 ] 2–, were obtained using 11 B double-quantum-filtered (DQF) J -resolved solid-state nuclear magnetic resonance (SSNMR) spectroscopy. Our results show that the magnitude of the DQF J splitting is influenced by both the crystallographic symmetry of the system and the presence of dynamics. The splittings are amplified by a factor of 3 as compared to the corresponding theoretical J coupling constants for cases where (1) there is an absence of dynamics but the boron pairs are crystallographically equivalent or (2) the boron pairs are crystallographically inequivalent but are rendered magnetically equivalent on the time scale of the experiment due to dynamic disorder, which was identified by 11 B and 13 C SSNMR experiments. Consequently, molecular motions need to be taken into consideration when interpreting the results of DQF J -resolved experiments, and conversely, these experiments may be used to identify dynamic disorder. Variable-temperature NMR data support the notion of three different motional processes with correlation times ranging from 10 2 to 10 6 s –1 over the temperature range of 248–306 K. When molecular motion and crystallographic symmetry are both accounted for, the J ( 11 B, 11 B) coupling constants for various [B 2 (CN) 6 ] 2– salts were measured to range from 29.4 to 35.8 Hz, and their electronic origins were determined using natural localized molecular orbital and natural bond orbital analyses. The coupling constants were found to strongly correlate to the hybridization states of the boron orbitals that form the B–B bonds and to the strength of the B–B bonds. This study provides a novel tool to study dynamics in ordered and disordered solids and provides new perspectives on electron-precise dianionic diboranes featuring two-center–two-electron bonds in the context of related compounds featuring multiply and singly bonded boron spin pairs.

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 score0.038
Threshold uncertainty score0.527

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 studies0.0000.001
Scholarly communication0.0000.000
Open science0.0010.000
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 head0.272
Teacher spread0.268 · 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

Citations19
Published2017
Admission routes2
Has abstractyes

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