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Record W3064676851 · doi:10.1039/d0cp03565c

Electron spin polarization transfer induced by triplet–radical interactions in the weakly coupled regime

2020· article· en· W3064676851 on OpenAlexafffund
Maria Giulia Dal Farra, Caterina Martin, Elisabetta Bergantino, Yuri E. Kandrashkin, Art van der Est, Marilena Di Valentin

Bibliographic record

VenuePhysical Chemistry Chemical Physics · 2020
Typearticle
Languageen
FieldBiochemistry, Genetics and Molecular Biology
TopicElectron Spin Resonance Studies
Canadian institutionsCanadian Sleep SocietyBrock University
FundersNatural Sciences and Engineering Research Council of CanadaUniversità degli Studi di Padova
KeywordsNeuroglobinNitroxide mediated radical polymerizationElectronChemistryElectron transferTriplet stateSpin polarizationPolarization (electrochemistry)RadicalPorphyrinSpin (aerodynamics)PhotochemistryAtomic physicsChemical physicsExcited statePhysicsQuantum mechanicsPhysical chemistryRadical polymerization

Abstract

fetched live from OpenAlex

We report the observation of electron spin polarization transfer from the triplet state of a porphyrin to a weakly coupled nitroxide radical in a mutant of human neuroglobin (NGB). The native iron-containing heme substrate of NGB has been substituted with Zn(ii) protoporphyrin IX and the nitroxide has been attached via site-directed spin labeling to the Cys120 residue. A reference synthetic polypeptide with free base tetraphenylporphyrin and a nitroxide bound to it is also studied. In both systems the nitroxide and the porphyrin are held at a fixed distance of approximately 2.4 nm. The transient EPR data of the NGB sample show that the triplet state of Zn(ii) protoporphyrin acquires significant net polarization, which is attributed to the dynamic Jahn-Teller effect. As the spin polarization of the protoporphyrin triplet state decays, a polarized EPR signal of the nitroxide arises. In contrast, the free base porphyrin in the reference polypeptide does not acquire net polarization and no polarization of the nitroxide label is observed. This is likely a result of the fact that the porphyrin is not Jahn-Teller active because of its lower symmetry. A perturbation theory treatment suggests that in the NGB sample, the polarization of the radical occurs by the transfer of net polarization from the triplet state. This process is also enhanced by the spectral broadening caused by the back and forth transitions associated with the dynamic Jahn-Teller effect. We propose that the novel transfer of polarization to the radical could be exploited to enhance the sensitivity of light-induced dipolar spectroscopy experiments.

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 categoriesMeta-epidemiology (narrow)
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 score1.000

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 studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
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 head0.013
GPT teacher head0.271
Teacher spread0.258 · 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

Citations29
Published2020
Admission routes2
Has abstractyes

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