Single-Molecule Solvation-Shell Sensing

被引：85

作者：

Leary, E. ^{[1
]}

Hobenreich, H. ^{[1
]}

Higgins, S. J. ^{[1
]}

van Zalinge, H. ^{[1
]}

Haiss, W. ^{[1
]}

Nichols, R. J. ^{[1
]}

Finch, C. M. ^{[2
]}

Grace, I. ^{[2
]}

Lambert, C. J. ^{[2
]}

McGrath, R. ^{[3
]}

Smerdon, J. ^{[3
]}

机构：

[1] Univ Liverpool, Dept Chem, Liverpool L69 7ZD, Merseyside, England

[2] Univ Lancaster, Dept Phys, Lancaster LA1 4YB, England

[3] Univ Liverpool, Dept Phys, Liverpool L69 7ZE, Merseyside, England

来源：

PHYSICAL REVIEW LETTERS | 2009年 / 102卷 / 08期

基金：

英国工程与自然科学研究理事会;

关键词：

ELECTRON-TRANSFER; CONDUCTANCE; TRANSPORT; CONDUCTIVITY; RESISTANCE; COMPLEXES; JUNCTIONS; PROTEINS; DEVICES; STATE;

D O I：

10.1103/PhysRevLett.102.086801

中图分类号：

O4 [物理学];

学科分类号：

0702 ;

摘要：

We present a new route to single-molecule sensing via solvation shells surrounding a current-carrying backbone molecule. As an example, we show that the presence of a water solvation shell "gates" the conductance of a family of oligothiophene-containing molecular wires, and that the longer the oligothiophene, the larger is the effect. For the longest example studied, the molecular conductance is over 2 orders of magnitude larger in the presence of a shell comprising just 10 water molecules. A first principles theoretical investigation of electron transport through the molecules, using the nonequilibrium Green's function method, shows that water molecules interact directly with the thiophene rings, significantly shifting transport resonances and greatly increasing the conductance. This reversible effect is confirmed experimentally through conductance measurements performed in the presence of moist air and dry argon.

引用

页数：4

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