ArticleProceedings of the National Academy of Sciences of the United States of America2019
Transition from stochastic events to deterministic ensemble average in electron transfer reactions revealed by single-molecule conductance measurement.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2019. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 13 papers.
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13 citing papers in PubMed, 71 citations in OpenAlex.
- Quantifying the Characteristic Turnover Frequency of an Individual Redox Enzyme via Real-Time Electrical Transduction of Catalytic Events in a Label-Free Single-Protein Junction.Journal of the American Chemical Society · 2026Article
- Fingerprint Recognition Based on Molecular-Scale Conductance Response via Electrochemically Gated Quantum Tunnelling.Sensors (Basel, Switzerland) · 2026Article
- Photoelectrochemistry of Redox-Active Self-Assembled Monolayers Formed on n-Si/Au Nanoparticle Photoelectrodes.Langmuir : the ACS journal of surfaces and colloids · 2024Article
- Single-molecule electrochemical imaging resolves the midpoint potentials of individual fluorophores on nanoporous antimony-doped tin oxide.Chemical science · 2024Article
- Total variation denoising-based method of identifying the states of single molecules in break junction data.Discover nano · 2024Article
- Large Mechanosensitive Thermoelectric Enhancement in Metallo-Organic Magnetic Molecules.Nano letters · 2023Article
- Generic dynamic molecular devices by quantitative non-steady-state proton/water-coupled electron transport kinetics.Proceedings of the National Academy of Sciences of the United States of America · 2023Article
- Scaling of quantum interference from single molecules to molecular cages and their monolayers.Proceedings of the National Academy of Sciences of the United States of America · 2022Article
- Electrochemically controlled rectification in symmetric single-molecule junctions.Proceedings of the National Academy of Sciences of the United States of America · 2022Article
- Stochasticity in Single-Entity Electrochemistry.Current opinion in electrochemistry · 2021Article
- Creating a regular array of metal-complexing molecules on an insulator surface at room temperature.Nature communications · 2020Article
- A Chemically Soldered Polyoxometalate Single-Molecule Transistor.Angewandte Chemie (International ed. in English) · 2020Article
- Fermi level-tuned optics of graphene for attocoulomb-scale quantification of electron transfer at single gold nanoparticles.Nature communications · 2019Article
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Authors and funding
8 authors at 4 institutions in 3 countries.
Funding
No grant is acknowledged in the PubMed record.
Abstract
Electron transfer reactions can now be followed at the single-molecule level, but the connection between the microscopic and macroscopic data remains to be understood. By monitoring the conductance of a single molecule, we show that the individual electron transfer reaction events are stochastic and manifested as large conductance fluctuations. The fluctuation probability follows first-order kinetics with potential dependent rate constants described by the Butler-Volmer relation. Ensemble averaging of many individual reaction events leads to a deterministic dependence of the conductance on the external electrochemical potential that follows the Nernst equation. This study discloses a systematic transition from stochastic kinetics of individual reaction events to deterministic thermodynamics of ensemble averages and provides insights into electron transfer processes of small systems, consisting of a single molecule or a small number of molecules.
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