Regulating a Benzodifuran Single Molecule Redox Switch via Electrochemical Gating and Optimization of Molecule/Electrode Coupling

被引:96
作者
Li, Zhihai [1 ]
Li, Hui [2 ]
Chen, Songjie [2 ]
Froehlich, Toni [3 ,4 ]
Yi, Chenyi [2 ]
Schoenenberger, Christian [3 ,4 ]
Calame, Michel [3 ,4 ]
Decurtins, Silvio [2 ]
Liu, Shi-Xia [2 ]
Borguet, Eric [1 ]
机构
[1] Temple Univ, Dept Chem, Philadelphia, PA 19122 USA
[2] Univ Bern, Dept Chem & Biochem, Bern, Switzerland
[3] Univ Basel, Dept Phys, CH-4056 Basel, Switzerland
[4] Univ Basel, Swiss Nanosci Inst, Basel, Switzerland
基金
瑞士国家科学基金会; 美国国家科学基金会;
关键词
CHARGE-TRANSPORT; ELECTRICAL CONDUCTANCE; PHOTOPHYSICAL PROPERTIES; JUNCTIONS; TRANSISTOR; RESISTANCE; CONTACTS;
D O I
10.1021/ja5034606
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
We report a novel strategy for the regulation of charge transport through single molecule junctions via the combination of external stimuli of electrode potential, internal modulation of molecular structures, and optimization of anchoring groups. We have designed redox-active benzodifuran (BDF) compounds as functional electronic units to fabricate metal-molecule-metal (m-M-m) junction devices by scanning tunneling microscopy (STM) and mechanically controllable break junctions (MCBJ). The conductance of thiol-terminated BDF can be tuned by changing the electrode potentials showing clearly an off/on/off single molecule redox switching effect. To optimize the response, a BDF molecule tailored with carbodithioate (-CS2-) anchoring groups was synthesized. Our studies show that replacement of thiol by carbodithioate not only enhances the junction conductance but also substantially improves the switching effect by enhancing the on/off ratio from 2.5 to 8.
引用
收藏
页码:8867 / 8870
页数:4
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