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Record W4320713005 · doi:10.1021/jacs.2c10915

Triangulating Dopant-Level Mn(II) Insertion in a Cs<sub>2</sub>NaBiCl<sub>6</sub>Double Perovskite Using Magnetic Resonance Spectroscopy

2023· article· en· W4320713005 on OpenAlexafffund
Abhoy Karmakar, Guy M. Bernard, Arkadii Pominov, Tarnuma Tabassum, Raj Chaklashiya, Songi Han, Sheetal Jain, Vladimir K. Michaelis

Bibliographic record

VenueJournal of the American Chemical Society · 2023
Typearticle
Languageen
FieldEngineering
TopicPerovskite Materials and Applications
Canadian institutionsUniversity of Alberta
FundersAlberta InnovatesNatural Sciences and Engineering Research Council of CanadaCanada Research Chairs
KeywordsElectron paramagnetic resonanceChemistryHyperfine structureElectron nuclear double resonancePerovskite (structure)DopantDopingCrystallographyParamagnetismSpectroscopyOctahedral symmetryNuclear magnetic resonanceCondensed matter physicsIonAtomic physics

Abstract

fetched live from OpenAlex

Lead-free metal halide double perovskites are gaining increasing attention for optoelectronic applications. Specifically, doping metal halide double perovskites using transition metals enables broadband tailorability of the optical bandgap for these emerging semiconducting materials. One candidate material is Mn(II)-doped Cs 2 NaBiCl 6, but the nature of Mn(II) insertion on chemical structure is poorly understood due to low Mn loading. It is critical to determine the atomic-level structure at the site of Mn(II) incorporation in doped perovskites to better understand the structure–property relationships in these materials and thus to advance their applicability to optoelectronic applications. Magnetic resonance spectroscopy is uniquely qualified to address this, and thus a comprehensive three-pronged strategy, involving solid-state nuclear magnetic resonance (NMR), high-field dynamic nuclear polarization (DNP), and electron paramagnetic resonance (EPR) spectroscopies, is used to identify the location of Mn(II) insertion in Cs 2 NaBiCl 6 . Multinuclear ( 23 Na, 35 Cl, 133 Cs, and 209 Bi) one-dimensional (1D) magnetic resonance spectra reveal a low level of Mn(II) incorporation, with select spins affected by paramagnetic relaxation enhancement (PRE) induced by Mn(II) neighbors. EPR measurements confirm the oxidation state, octahedral symmetry, and low doping levels of the Mn(II) centers. Complementary EPR and NMR measurements confirm that the cubic structure is maintained with Mn(II) incorporation at room temperature, but the structure deviates slightly from cubic symmetry at low temperatures (<30 K). HYperfine Sublevel CORrelation (HYSCORE) EPR spectroscopy explores the electron–nuclear correlations of Mn(II) with 23 Na, 133 Cs, and 35 Cl. The absence of 209 Bi correlations suggests that Bi centers are replaced by Mn(II). Endogenous DNP NMR measurements from Mn(II) → 133 Cs (<30 K) reveal that the solid effect is the dominant mechanism for DNP transfer and supports that Mn(II) is homogeneously distributed within the double-perovskite structure.

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 score0.023
Threshold uncertainty score0.802

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.001
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 head0.020
GPT teacher head0.250
Teacher spread0.230 · 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

Citations37
Published2023
Admission routes2
Has abstractyes

Explore more

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