Charge Localization in Isolated Mixed-Valence Complexes: An STM and Theoretical Study

被引：86

作者：

Lu, Yuhui ^{[2
]}

Quardokus, Rebecca ^{[1
]}

Lent, Craig S. ^{[2
]}

Justaud, Frederic ^{[3
]}

Lapinte, Claude ^{[3
]}

Kandel, S. Alex ^{[1
]}

机构：

[1] Univ Notre Dame, Dept Chem & Biochem, Notre Dame, IN 46556 USA

[2] Univ Notre Dame, Dept Elect Engn, Notre Dame, IN 46556 USA

[3] Univ Rennes 1, CNRS, UMR 6226, F-35042 Rennes, France

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2010年 / 132卷 / 38期

基金：

美国国家科学基金会;

关键词：

SCANNING-TUNNELING-MICROSCOPY; QUANTUM CELLULAR-AUTOMATA; DENSITY-FUNCTIONAL THEORY; ELECTRON-TRANSFER; MOLECULAR ELECTRONICS; AU(111); BENZENE; SYSTEMS; FIELD; COUNTERIONS;

D O I：

10.1021/ja105958p

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

{Cp-star(dppe)Fe(C C-)}(2)(1,3-C6H4) is studied both as a neutral molecule, Fe(II)-Fe(II), and as a mixed-valence complex, Fe(II)-Fe(III). Scanning tunneling microscopy (STM) is used to image these species at 77 K under ultrahigh-vacuum conditions. The neutral molecule Fe(II)-Fe(II) has a symmetric, "dumbbell" appearance in STM images, while the mixed-valence complex Fe(II)-Fe(III) demonstrates an asymmetric, bright-dim double-dot structure. This asymmetry results from localization of the electron to one of the iron-ligand centers, a result which is confirmed through comparison to theoretical STM images calculated using constrained density-functional theory (CDFT). The observation of charge localization in mixed-valence complexes outside of the solution environment opens up new avenues for the control and patterning of charge on surfaces, with potential applications in smart materials and molecular electronic devices.

引用

页码：13519 / 13524

页数：6

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