Functional (Supra)Molecular Nanostructures - ruben-group

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Habilitation Dr. Mario Ruben ULP Strasbourg The Ag I ions are dicoordinated in an approximately linear coordination manner with d(Ag-N) = 2.130(12)-2.228(14) Å; α(N-Ag-N) = 166.4(7)° and 168.8(8)°, and interconnect each tetranuclear [Fe II 4B4] 8+ unit to four neighbouring units each time by two pyridine-Ag I - pyridine bridges. Following this coordination scheme, an infinite coordination polymer is generated as a meander-like interwoven, two-dimensional network. Within this “brickwall”- like framework, the [Fe II 4B4] 8+ -units are aligned in rows 2.15 nm apart, while the distance between two neighbouring “brickwalls” is around 1.56 nm (Figure 7). The represented results show that self-assembly processes using suitably designed molecular components can be implemented to construct the metallo-supramolecular brick modules [Fe4A4] 8+ (1) and, [Fe4B4] 8+ (2), displaying both the structural prerequisites which enable 1 and 2 to undergo a second self-assembly process. This second process leads in both cases to a hierarchically ordered, either one-dimensional “column”-like {-[Fe II 4A4]-(La III )}n 11+ (3), or two-dimensional “brickwall”-like {-[Fe II 4B4]-(Ag I )4}n 12+ (4) architectures. The variation of the properties (herein magnetic) of the molecular architectures depending on progressing hierarchical levels of complexation will be shown in detail in chapter 6.1. 15
Habilitation Dr. Mario Ruben ULP Strasbourg 4.2. Surface-assisted Self-Assembly and Coordination A) Surface deposition of pre-assembled supramolecules (in collaboration with Prof. P. Müller, University of Erlangen, Germany) The controlled arrangement of supramolecular [2x2] metal ion arrays on surfaces might provide materials with addressable functional subunits smaller than the conventionally studied quantum dots. The sub-nanometer exploitation of the molecular properties requires a precise control of the positioning of the [2x2] metal ion arrays onto the surface. Such positioning processes might be steered by templating effects directed by weak van-der Waals interacting with the underlying substrate lattices. Successful attempts of the preparation of closely- packed, highly ordered monolayers of grid-like [2x2] metal ion arrays on pyrolytic graphite were reported before. Furthermore, it was shown, that single molecules within the full- coverage monolayer could be addressed destructively by removal with STM-tip manipulations. [4] Ongoing work towards low-dimensional arrangements of [Co II 4L 1 4] 8+ metal ion arrays has shown that in very dilute conditions, the supramolecules get trapped along the step edges of the highly ordered pyrolytic graphite after sputtering 10 -4 mol l -1 in acetonitrile solutions. Using this technique, it was possible to obtain continuous 1D chains of several hundred nanometers as well as 2D arrays of densely packed grid-like supramolecules depending on the concentration (Figure 8). The ordered 2D structures form spontaneously, growing outward from single nucleation points. This process might be viewed as the 2D equivalent of a crystallization process. Figure 8. STM-images of samples generated by sputtering of acetonitrile solutions of [Co II 4L4] 8+ grid-like complexes at room temperature on graphite; left) an isolated molecule; centre) at low concentrations, the [Co II 4L4] 8+ complexes are ordered along graphite steps into 1D chains; right) following the same protocol, at higherconcentrations, 2D arrangements made from [Co II 4L4] 8+ metal ion arrays could be obtained. 16
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