Observing Single, Heterogeneous, One-Electron Transfer Reactions

被引:38
|
作者
Zaleski, Stephanie [1 ]
Cardinal, M. Fernanda [1 ]
Klingsporn, Jordan M. [1 ]
Van Duyne, Richard P. [1 ,2 ,3 ]
机构
[1] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
[2] Northwestern Univ, Dept Biomed Engn, Evanston, IL 60208 USA
[3] Northwestern Univ, Program Appl Phys, Evanston, IL 60208 USA
来源
JOURNAL OF PHYSICAL CHEMISTRY C | 2015年 / 119卷 / 50期
基金
美国国家科学基金会;
关键词
SURFACE-ENHANCED RAMAN; MOLECULE SERS; SILVER NANOPARTICLES; REDOX MOLECULES; HOT-SPOTS; SPECTROSCOPY; SCATTERING; ELECTROCHEMISTRY; MICROSCOPY; METAL;
D O I
10.1021/acs.jpcc.5b10652
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Understanding electrochemical events on the single-molecule level is crucial for fields such as catalysis and biological system. A variety of techniques exist to study the electrochemistry of single molecules, but few provide correlated chemical information. Herein, we study the electrochemistry of rhodamine 6G in nonaqueous conditions and demonstrate the first statistic electrochemical single-molecule SERS (EC-SMSERS) proof of single-electron transfer events. We find that the distribution of reduction events is broader than that hi a bulk electrochemical experiment. The distribution of the reduction potentials can be explained by molecular reorientation and variations of the local surface rite or chemical potential of the Ag nanoparticle. Our results contribute toward understanding electrochemical behavior of single molecules on the nanoscale monitored by SERS and the ultimate goal of controlling single-electron transfer processes.
引用
收藏
页码:28226 / 28234
页数:9
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