Exploring Bridges between Quantum Transport and Electrochemistry. I.
2016
In this work we present a theoretical connection between the Landauer picture utilized in quantum transport and the Gerischer picture utilized in electrochemistry. A comprehensive analysis of the single-particle picture and total energy picture in electrochemistry is presented, followed by derivation of electron transfer rates utilizing the nonequilibrium Green’s function formalism. Correlations are also made with the Marcus–Hush theoretical approach more often utilized in electrochemistry. The analysis is limited to tunneling (also called outer-sphere) electrochemical reactions. In general, it is expected that this work will serve to further bridge the diverse condensed matter and chemistry foundations inherent to interfacial electrochemistry.
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