A Three-Step Kinetic Model for Electrochemical Charge Transfer in the Hopping Regime

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• 作者：Xing Yin ; Emil Wierzbinski ; Hao Lu ; Silvia Bezer ; Arnie R. de Leon ; Kathryn L. Davis ; Catalina Achim ; David H. Waldeck
• 刊名：Journal of Physical Chemistry A
• 出版年：2014
• 出版时间：September 4, 2014
• 年：2014
• 卷：118
• 期：35
• 页码：7579-7589
• 全文大小：496K
• ISSN：1520-5215

文摘

Single-step nonadiabatic electron tunneling models are widely used to analyze electrochemical rates through self-assembled monolayer films (SAMs). For some systems, such as nucleic acids, long-range charge transfer can occur in a 鈥渉opping鈥?regime that involves multiple charge transfer events and intermediate states. This report describes a three-step kinetic scheme to model charge transfer in this regime. Some of the features of the three-step model are probed experimentally by changing the chemical composition of the SAM. This work uses the three-step model and a temperature dependence of the charge transfer rate to extract the charge injection barrier for a SAM composed of a 10-mer peptide nucleic acid that operates in the hopping regime.