Interfacial Screening in Ultrafast Voltammetry: A Theoretical Study of Redox-Active Monolayers
Bibliographic record
Abstract
The impact of interfacial screening on electron transfer (ET) at ultrashort time scales is theoretically investigated on redox active monolayers by linear sweep voltammetry (LSV). The charging current associated with the nanosecond screening process is an important experimental determinant in finding both the reorganization energy (λ) and electronic coupling (|M|) through ultrafast methods. On the one hand, time dependent decay of the charging current mitigates its impact on the current contribution from faradaic processes, while on the other hand, allowing substantial decay translates into a reduced upper-bound of applicable scan rates, which are crucial for ultrafast characterization. Analysis of the decay in the charging current suggests that the desired screening may be achieved for relatively weakly coupled systems within the charging time constant. For weakly coupled systems, the scan rate corresponding to nanoscale charging time constants appears to be suitable for the ultrafast investigation of ET characteristics. Moreover, the level of screening achieved at nanosecond decay times is shown to change with the coverage of electrode surface by monolayers; which appears to be accompanied by sharp drops in the time constant during successive saturation of interfacial layers by supporting ions (SI). These observations are expected to help design electrochemical device systems with interfaces capable of high faradaic efficiency at ultrafast limits.
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.
Distilled classifier scores by category (both heads)
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.001 |
| Meta-epidemiology (narrow) | 0.001 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.001 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.001 |
| Scholarly communication | 0.000 | 0.001 |
| Open science | 0.001 | 0.001 |
| Research integrity | 0.001 | 0.001 |
| Insufficient payload (model declined to judge) | 0.001 | 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 source (direct Gemma or distilled Codex), 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".