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Record W3161116124 · doi:10.1002/cptc.202100048

The Sulfolene Protecting Group: Observation of a Direct Photoinitiated Cheletropic Ring Opening

2021· article· en· W3161116124 on OpenAlexaff
Anders B. Skov, Linnea M. Folkmann, Andrey E. Boguslavskiy, Anja Röder, Rune Lausten, Albert Stolow, Matthew S. Johnson, Michael Pittelkow, Ole John Nielsen, Theis I. Sølling, Thorsten Hansen

Bibliographic record

VenueChemPhotoChem · 2021
Typearticle
Languageen
FieldMaterials Science
TopicPhotochromic and Fluorescence Chemistry
Canadian institutionsJoint Attosecond Science LaboratoryNational Research Council CanadaUniversity of Ottawa
FundersLundbeckfonden
KeywordsRing (chemistry)Group (periodic table)ChemistryPhotochemistryOrganic chemistry

Abstract

fetched live from OpenAlex

Abstract Photolabile protecting groups offer synthetic routes with facile deprotection by photolysis, providing higher yields with less workup. Protecting groups producing only gaseous byproducts upon removal are particularly desirable as sustainable reagents. Cheletropic reactions provide just this combination of photocleavable groups with gaseous byproducts. However, only few protecting groups for cheletropic reactions have been described and little is known about their photochemistry and associated stereochemistry. Here we show that the sulfolene protecting group, used for diene protection and functionalization, can be photochemically removed. First, using TD‐DFT, we conclude that the photochemical ring‐opening occurs conrotatorily in a concerted process, consistent with the Woodward‐Hoffmann rules. Experimentally, we demonstrate that this process can be photoinitiated by radiation between 180 and 300 nm and confirm the proposed stereochemistry in solution. Using time‐resolved photoelectron spectroscopy, we determine that the first steps in the photochemical ring‐opening of sulfolene occur on ultrafast timescales (≤84 fs), consistent with a fully concerted process. Our findings expand applications of the sulfolene protecting group and promise an easy strategy for control of cis‐trans isomerization.

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)0.001
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 score0.004
Threshold uncertainty score0.639

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.001
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 head0.022
GPT teacher head0.241
Teacher spread0.219 · 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

Citations3
Published2021
Admission routes1
Has abstractyes

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