Modulated Intermolecular Interactions in Ferrocenylalkanethiolate Self-Assembled Monolayers on Gold
Bibliographic record
Abstract
Redox-labeled self-assembled monolayers (SAMs) on gold are excellent model systems for the study of long-range electron transfer processes at electrolyte–electrode interfaces, particularly the distance and reorganization energy dependences. In this work, we have shown that the intermolecular interaction among redox centers is in fact a crucial factor in the overall, nonideal electrochemical response of ferrocenylalkanethiolate SAMs on gold. In both single-component and high-ratio binary monolayers of 11-ferrocenyl-1-undecanethiol (FcC11SH), the two distinct pairs of redox peaks are corresponding to rather moderate differences in the packing densities of the two structural domains. We have discovered that the redox peak at lower potential becomes narrower and higher when organic solvents (nitrobenzene or octanol) are added to the aqueous electrolyte, while the peak at the higher potentials is barely influenced. On the basis of the Frumkin isotherm, we have obtained the intermolecular interaction parameters in the different structural domains of the monolayers by fitting the experimental data. The results showed that the intermolecular interaction in the FcC11S–Au SAMs can change from repulsion to attraction upon adding organic solvent in the aqueous electrolyte. It is suggested that the solvent perturbation to the SAM structure at monolayer/electrolyte interface induces remarkable change in the intermolecular interactions and therefore modulates the observed electrochemical responses from nonideal to nearly ideal.
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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 | 0.000 |
| 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 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".