Functional (Supra)Molecular Nanostructures - ruben-group

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Habilitation Dr. Mario Ruben ULP Strasbourg Figure 14: Schematic representation and STM image of the coordination mode the infinite rectangular coordination network on Cu(100) surface with dimeric Fe2-units at the crossing points of the grid-like network. The Fe-O bond distances estimated from STM data are close to that of bulk materials (d(Fe-O)= 1.9-2.3 Å) [12] and the metal centers are held at a metal-metal distance of about d(Fe-Fe) = 5 Å. However, the observation of sometimes elongated Fe-O bonds might be indicative of a situation in which both ligand and metal centres are in close contact with the Cu(100) surface, which is then obviously acting a template. Thus, the underlying crystal lattice as well as the conduction band of the substrate might interfere structurally as well as electronically in the final positioning of the involved metal atoms relative to the organic ligands. However, looking at the distinct M2L4/2-stocheometry of the dimeric Fe2-nods, it seems reasonable to reckon that the principle of electro-neutrality is still persisting also under interfacial conditions. Such a view would lead to the definition of two Fe(II) ions surrounded by four deprotonated, negatively charged carboxylic <strong>group</strong>s. The formation of such electro- neutral 4+/4- units will depend critically on the smoothness of the deprotonation reaction, during which four carboxylic protons have to be reduced to two mole Hydrogen under simultaneous oxidation of the two Iron(0) centers. The gaseous Hydrogen could easily migrate into the UHV environment so favoring the accomplishment of the redox reaction. The local electro-neutrality around the dimeric Fe2-knots may also explain the high thermal stability of the 2D networks up to 500 K (although they are not stable in the presence of ambient gases). The further elucidation of the coordination characteristics of metal centers in close contact to metallic surfaces (coordination number, redox- and spin- state, metal-metal interactions, mirror charges, etc.) is under investigation and the results might advent a new 23
Habilitation Dr. Mario Ruben ULP Strasbourg branch of “surface-assisted” metal coordination chemistry (maybe as extension of the more bulk- and solution-based, conventional “Werner-type” one). Together with other molecule- dealing STM-based surface manipulations (e.g. C-C bond formation, surface chirality) [13] and new approaches towards nano-magnetism (e.g. spin-polarized STM), [14] such “surface- assisted” coordination chemistry might constitute part of the future tool kit needed to put into reality directed construction and controlled manipulation of functional interfaces and operational surfaces. 24
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Functional (Supra)Molecular Nanostructures - ruben-group

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