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Record W2300887109 · doi:10.1021/jacs.5b12181

Maximizing Electron Exchange in a [Fe<sub>3</sub>] Cluster

2016· article· en· W2300887109 on OpenAlexfundno aff
Raúl Hernández Sánchez, Amymarie K. Bartholomew, Tamara M. Powers, Gabriel Ménard, Theodore A. Betley

Bibliographic record

VenueJournal of the American Chemical Society · 2016
Typearticle
Languageen
FieldMaterials Science
TopicMagnetism in coordination complexes
Canadian institutionsnot available
FundersNational Institute of General Medical SciencesNatural Sciences and Engineering Research Council of CanadaConsejo Nacional de Ciencia y TecnologíaNational Institutes of HealthHarvard UniversityNovartisU.S. Department of Energy
KeywordsChemistryCluster (spacecraft)ElectronElectron exchangeChemical physicsNuclear physicsIonOrganic chemistryPhysics

Abstract

fetched live from OpenAlex

The one-electron reduction of ((tbs)L)Fe₃(thf)¹ furnishes [M][((tbs)L)Fe₃] ([M]⁺ = [(18-C-6)K(thf)₂]⁺ (1, 76%) or [(crypt-222)K]⁺ (2, 54%)). Upon reduction, the ligand (tbs)L⁶⁻ rearranges around the triiron core to adopt an almost ideal C₃-symmetry. Accompanying the ((tbs)L) ligand rearrangement, the THF bound to the neutral starting material is expelled, and the Fe-Fe distances within the trinuclear cluster contract by ∼0.13 Å in 1. Variable-temperature magnetic susceptibility data indicates a well-isolated S = 11/2 spin ground state that persists to room temperature. Slow magnetic relaxation is observed at low temperature as evidenced by the out-of-phase (χ(M)″) component of the alternating current (ac) magnetic susceptibility data and by the appearance of hyperfine splitting in the zero-field ⁵⁷Fe Mössbauer spectra at 4.2 K. Analysis of the ac magnetic susceptibility yields an effective spin reversal barrier (U(eff)) of 22.6(2) cm⁻¹, nearly matching the theoretical barrier of 38.7 cm⁻¹ calculated from the axial zero-field splitting parameter (D = -1.29 cm⁻¹) extracted from the reduced magnetization data. A polycrystalline sample of 1 displays three sextets in the Mössbauer spectrum at 4.2 K (H(ext) = 0) which converge to a single six-line pattern in a frozen 2-MeTHF glass sample, indicating a unique iron environment and thus strong electron delocalization. The spin ground state and ligand rearrangement are discussed within the framework of a fully delocalized cluster exhibiting strong double and direct exchange interactions.

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: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.002
Threshold uncertainty score0.005

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 studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.000
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 head0.012
GPT teacher head0.247
Teacher spread0.236 · 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 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

Citations56
Published2016
Admission routes1
Has abstractyes

Explore more

Same venueJournal of the American Chemical SocietySame topicMagnetism in coordination complexesFrench-language works237,207