1] Peter Grünberg Institut (PGI-3), Forschungszentrum Jülich, 52425 Jülich, Germany [2] Jülich Aachen Research Alliance (JARA)-Fundamentals of Future Information Technology, 52425 Jülich, Germany [3].
Institut für Physik, Karl-Franzens-Universität Graz, Graz 8010, Austria.
Nat Commun. 2014 Apr 16;5:3685. doi: 10.1038/ncomms4685.
Although geometric and electronic properties of any physical or chemical system are always mutually coupled by the rules of quantum mechanics, counterintuitive coincidences between the two are sometimes observed. The coadsorption of the organic molecules 3,4,9,10-perylene tetracarboxylic dianhydride and copper-II-phthalocyanine on Ag(111) represents such a case, since geometric and electronic structures appear to be decoupled: one molecule moves away from the substrate while its electronic structure indicates a stronger chemical interaction, and vice versa for the other. Our comprehensive experimental and ab-initio theoretical study reveals that, mediated by the metal surface, both species mutually amplify their charge-donating and -accepting characters, respectively. This resolves the apparent paradox, and demonstrates with exceptional clarity how geometric and electronic bonding parameters are intertwined at metal-organic interfaces.
尽管任何物理或化学系统的几何和电子性质总是通过量子力学的规则相互耦合，但有时也会观察到两者之间违反直觉的巧合。有机分子 3,4,9,10-苝四羧酸二酐和铜 II-酞菁在 Ag(111)上的共吸附就是这样一个例子，因为几何和电子结构似乎是解耦的：一个分子从衬底上移开，而其电子结构表明更强的化学相互作用，而另一个分子则相反。我们的综合实验和从头算理论研究表明，通过金属表面，两种物质都相互放大了它们的供体和受体特性。这解决了明显的悖论，并以非凡的清晰度展示了金属-有机界面上的几何和电子键参数是如何交织在一起的。
