Local density of states effects at the metal-molecule interfaces in amolecular device

被引:104
作者
Boyen, HG [1 ]
Ziemann, P
Wiedwald, U
Ivanova, V
Kolb, DM
Sakong, S
Gross, A
Romanyuk, A
Büttner, M
Oelhafen, P
机构
[1] Univ Ulm, Abt Festkorperphys, D-89069 Ulm, Germany
[2] Univ Ulm, Abt Elektrochem, D-89069 Ulm, Germany
[3] Univ Ulm, Abt Theoret Chem, D-89069 Ulm, Germany
[4] Univ Basel, Inst Phys, CH-4056 Basel, Switzerland
关键词
D O I
10.1038/nmat1607
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
Clarifying the nature of interactions between metal electrodes and organic molecules still represent one of the challenging problems in molecular electronics that needs to be solved in order to optimize electron transport through a molecular device. For this purpose, electronic properties at metal - molecule interfaces were studied by combining experimental and theoretical methods. Applying a novel electrochemical approach, strictly two-dimensional Pd islands were prepared on top of 4-mercaptopyridine self-assembled monolayers (4MP-SAMs) which, in turn, were deposited on (111)-oriented Au single crystals. Electron spectroscopy together with density functional theory calculations revealed strong interactions between the molecules and the islands due to Pd-N bonds, resulting in a drastically reduced density of states ( DOS) at the Fermi level E-F for a nearly closed Pd monolayer, and even non-metallic properties for nanometre-sized islands. Similarly, a significantly reduced DOS at EF was observed for the topmost Au layer at the Au-SAM interface due to Au-S interactions, suggesting that these effects are rather general.
引用
收藏
页码:394 / 399
页数:6
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