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Record W2327383095 · doi:10.1021/cg3009255

A Pressure Induced Structural Dichotomy in Isostructural Bis-1,2,3-thiaselenazolyl Radical Dimers

2012· article· en· W2327383095 on OpenAlexafffund
Kristina Lekin, Alicea A. Leitch, John S. Tse, Xuezhao Bao, Richard A. Secco, Serge Desgreniers, Yasuo Ohishi, Richard T. Oakley

Bibliographic record

VenueCrystal Growth & Design · 2012
Typearticle
Languageen
FieldMaterials Science
TopicOrganic and Molecular Conductors Research
Canadian institutionsUniversity of OttawaWestern UniversityUniversity of WaterlooUniversity of Saskatchewan
FundersNatural Sciences and Engineering Research Council of CanadaCanada Research ChairsGovernment of Canada
KeywordsCrystallographyIsostructuralChemistryDimerMonoclinic crystal systemCrystal structureBond lengthMolecular geometryDiamond anvil cellChemical physicsDiffractionMoleculeOptics

Abstract

fetched live from OpenAlex

The pressure dependence of the crystal and molecular structure of the bis-1,2,3-thiaselenazolyl radical dimer [ 1b ] 2 has been investigated over the range 0–11 GPa by powder diffraction methods using synchrotron radiation and diamond anvil cell techniques. At ambient pressure, the dimer consists of a pair of radicals linked by a hypervalent 4-center 6-electron S---Se–Se---S σ-bond in an essentially coplanar arrangement. The dimers are packed in cross-braced slipped π-stack arrays running along the x -direction of the monoclinic (space group P 2 1 / c ) unit cell. Pressurization to 11 GPa causes the unit cell dimensions a and c to undergo a slow but uniform compression, while the b -axis is slightly elongated. There is virtually no change in the molecular structure or in the slipped π-stack crystal architecture. This behavior is in marked contrast to that of the isostructural radical dimer [ 1a ] 2, where the basal fluorine is replaced by hydrogen. Pressurization of this latter material induces a phase change near 4–5 GPa, characterized by a sharp contraction in a and c, and a correspondingly large increase in b . At the molecular level, the transition is associated with a buckling of the σ-bonded dimer to a more conventional π-bonded arrangement. Geometry optimized DFT band structure calculations on [ 1b ] 2 replicate the observed structural changes and indicate that compression widens both the valence and conduction bands but does not induce band gap closure until >13 GPa. This result is consistent with the measured thermal activation energy for conduction E act, which indicates that a metallic state requires pressures > 10 GPa.

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)0.001
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow), Insufficient payload (model declined to judge)
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 score0.021
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.001
Open science0.0010.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0020.000

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 head0.032
GPT teacher head0.276
Teacher spread0.244 · 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.

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

Citations16
Published2012
Admission routes2
Has abstractyes

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