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Record W4281694024 · doi:10.1002/cphc.202200188

Understanding the Deactivating/Activating Mechanisms in Three Optical Chemosensors Based on Crown Ether with Na<sup>+</sup>/K<sup>+</sup> Selectivity Using Quantum Chemical Tools

2022· article· en· W4281694024 on OpenAlexafffund
Manuel A. Treto‐Suárez, Eduardo Schott, Karel Mena Ulecia, Bryan D. Koivisto, Yoan Hidalgo‐Rosa, Dayán Páez‐Hernández, Ximena Zárate

Bibliographic record

VenueChemPhysChem · 2022
Typearticle
Languageen
FieldChemistry
TopicMolecular Sensors and Ion Detection
Canadian institutionsToronto Metropolitan UniversityUniversity of Toronto
FundersAlliance de recherche numérique du CanadaCompute Canada
KeywordsChemistryDensity functional theoryTime-dependent density functional theoryQuenching (fluorescence)LuminescencePhotochemistryFluorophoreSelectivityIntramolecular forceConformational isomerismExcited stateLone pairOscillator strengthFluorescenceMoleculeComputational chemistryMaterials scienceStereochemistrySpectral lineOrganic chemistryAtomic physics

Abstract

fetched live from OpenAlex

Abstract The optical properties and transduction mechanisms in three reported optical chemosensors based on crown ether with selectivity turn‐on luminescence toward Na + over K + , were investigated using Density Functional Theory/Time‐Dependent Density Functional Theory (DFT/TD‐DFT). The analysis of the structural stability of the conformers enables us to understand the optical properties of the sensors and their selectivity toward Na + . The UV‐Vis absorption and the radiative channels of the adiabatic S 1 excited state were assessed. In these reported sensors, the Photoinduced Electron Transfer (PET) from the nitrogen and the oxygen (O‐atoms of the substituted N‐phenylaza group) lone pairs to fluorophore groups lead to a nonradiative deactivation process in the fluorophore to p‐conjugated anilino‐1,2,3‐triazol ionophore. This Intramolecular Charge Transfer (ICT) deactivation produced the luminescence quenching in the free sensors and K + / C1 complexes. The Na + /sensor interaction produced a Chelation Enhanced Fluorescence (CHEF) due to the inhibition of the PET and ICT, which was confirmed via the calculated oscillator strength of the emission process. The K + /sensor interaction displayed the possibility of PET in C3 ; however, this fact was inconclusive to affirm the quenching of luminescence, the CHEF in C2 and C3 and the selectivity toward Na + over K + in these systems. For this reason, simulation of the absorption and emissions spectra (calculated oscillator strength), calculation of the kinetic parameters (in charge transfers and radiative deactivations process), analysis of the metal‐ligand interaction character, and the analysis of the structural stability of the conformers were determinant factors to understand the selectivity and the optical properties of these chemosensors. The results suggest that these theoretical tools can also be used to predict the optical properties and Na + /K + selectivity of optical chemosensors.

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 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 score0.289
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.001
Meta-epidemiology (narrow)0.0010.001
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0000.001
Science and technology studies0.0010.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.002
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 head0.055
GPT teacher head0.248
Teacher spread0.193 · 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

Citations5
Published2022
Admission routes2
Has abstractyes

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