Counting Single Redox Turnovers: Fluorogenic Antioxidant Conversion and Mass Transport Visualization via Single Molecule Spectroelectrochemistry
Bibliographic record
Abstract
We report herein the use of single molecule spectroelectrochemistry (SMS-EC) to optically detect electrochemically activated individual molecules of the redox-active, tocopherol-like fluorogenic probe H 2 B-PMHC. Single molecule detection combined with a fluorescence burst frequency analysis is shown to provide a most sensitive method to monitor subnanomolar concentrations of the electrochemically activated probe. By measuring changes in activated probe concentration over time and distance from a planar electrode, mass transport characteristics of a prototype infinite planar electrode system are retrieved as a showcase study. We show that fluorescence activation may be achieved under both oxidative (direct oxidation of H 2 B-PMHC) and reductive (via O 2 •- production) conditions. Our results conducted in organic solvents broaden the scope of electrochemical reactions that can be studied by SMS-EC. The methodology we describe may potentially aid the study of mass transport in systems with complex electrode geometries or hampered diffusion.
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How this classification was reachedexpand
Full frame distilled prediction
Teacher imitationNot 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.
Codex and Gemma teacher scores by category
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.000 | 0.000 |
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.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one teacher head, not a consensus.
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".