Metal Ion Complexation: A Route to 2 D Templates?

Feyter, Steven De; Abdel‐Mottaleb, M. S. A.; Schuurmans, Norbert; Verkuijl, Bas; Esch, Jan H. van; Feringa, Ben L.; Schryver, F. C. De

doi:10.1002/chem.200305424

Cited by 64 publications

(53 citation statements)

References 57 publications

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“…4B and 4E exhibit an internal structure, which resembles the arrangement of planar or extended stacking rows of bipyridine units in self-assembled monolayers. 97,98 In analogy to these reports we attribute the light grey rows in the high resolution STM images tentatively to the positions of the viologen moieties. The intermolecular distance between neighboring units, 0.43 nm (¼ O3 a Au sin 601) is too small to allow a plane-parallel arrangement to the substrate, but also too large for a perfect stacking structure.…”

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confidence: 78%

Two-dimensional assembly and local redox-activity of molecular hybrid structures in an electrochemical environment

et al. 2006

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The self-assembly and redox-properties of two viologen derivatives, N-hexyl-N 0 -(6-thiohexyl)-4,4 0 -bipyridinium bromide (HS-6V6-H) and N,N 0 -bis(6-thiohexyl)-4,4 0 -bipyridinium bromide (HS-6V6-SH), immobilized on Au(111)-(1 Â 1) macro-electrodes were investigated by cyclic voltammetry, surface enhanced infrared spectroscopy (SEIRAS) and in situ scanning tunneling microscopy (STM). Depending on the assembly conditions one could distinguish three different types of adlayers for both viologens: a low coverage disordered and an ordered ''striped'' phase of flat oriented molecules as well as a high coverage monolayer composed of tilted viologen moieties. Both molecules, HS-6V6-H and HS-6V6-SH, were successfully immobilized on Au(poly) nano-electrodes, which gave a well-defined redox-response in the lower pA-current range. An in situ STM configuration was employed to explore electron transport properties of single molecule junctions Au(T)|HS-6V6-SH(HS-6V6-H)|Au(S). The observed sigmoidal potential dependence, measured at variable substrate potential E S and at constant bias voltage (E T À E S ), was attributed to electronic structure changes of the viologen moiety during the one-electron reduction/re-oxidation process V 21 2 V 1d . Tunneling experiments in asymmetric, STM-based junctions Au(T)-S-6V6-H|Au(S) revealed current (i T )-voltage (E T ) curves with a maximum located at the equilibrium potential of the redox-process V 21 2 V 1d . The experimental i T À E T characteristics of the HS-6V6-H-modified tunneling junction were tentatively attributed to a sequential two-step electron transfer mechanism.

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confidence: 78%

Two-dimensional assembly and local redox-activity of molecular hybrid structures in an electrochemical environment

et al. 2006

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“…The generality of the effect suggests that it could play an important role in wide range of systems, for example, in controlling and enhancing charge transport at interfaces 12,38 , in influencing crystal growth 17 or the stability of colloidal solutions and emulsions 18 . In addition, this effect could also be exploited in the design and self-assembly of nanomaterials 39 and used to template nanostructures 16 .…”

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confidence: 99%

Water-induced correlation between single ions imaged at the solid–liquid interface

2014

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When immersed into water, most solids develop a surface charge, which is neutralized by an accumulation of dissolved counterions at the interface. Although the density distribution of counterions perpendicular to the interface obeys well-established theories, little is known about counterions' lateral organization at the surface of the solid. Here we show, by using atomic force microscopy and computer simulations, that single hydrated metal ions can spontaneously form ordered structures at the surface of homogeneous solids in aqueous solutions. The structures are laterally stabilized only by water molecules with no need for specific interactions between the surface and the ions. The mechanism, studied here for several systems, is controlled by the hydration landscape of both the surface and the adsorbed ions. The existence of discrete ion domains could play an important role in interfacial phenomena such as charge transfer, crystal growth, nanoscale self-assembly and colloidal stability.

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“…These processes will play a critical role in the so-called ''bottom-up'' strategy of nanofabrication. Therefore, understanding the organization of molecules on solid surfaces is important, both from a fundamental and applied perspective, for the construction of surface molecular nanostructures and nanodevices (3)(4)(5)(6)(7)(8)(9)(10)(11)(12)(13). A self-organized molecular pattern with control of structure and derived concomitant function could provide promising materials for the construction of nanodevices that cannot be prepared by conventional microfabrication.…”

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confidence: 99%

Mesoscopic self-organization of a self-assembled supramolecular rectangle on highly oriented pyrolytic graphite and Au(111) surfaces

Gong

Wan

Yuan

et al. 2005

Proc. Natl. Acad. Sci. U.S.A.

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A self-assembled supramolecular metallacyclic rectangle was investigated with scanning tunneling microscopy on highly oriented pyrolytic graphite and Au(111) surfaces. The rectangles spontaneously adsorb on both surfaces and self-organize into well ordered adlayers. On highly oriented pyrolytic graphite, the long edge of the rectangle stands on the surface, forming a 2D molecular network. In contrast, the face of the rectangle lays flat on the Au(111) surface, forming linear chains. The structures and intramolecular features obtained through high-resolution scanning tunneling microscopy imaging are discussed.metallacyclic macrocycle ͉ scanning tunneling microscopy ͉ molecular adlayer ͉ molecular orientation S elf-organization (1) and self-assembly (2) are critical and necessary processes in all living organisms and are of ever increasing importance in chemistry and material science. These processes will play a critical role in the so-called ''bottom-up'' strategy of nanofabrication. Therefore, understanding the organization of molecules on solid surfaces is important, both from a fundamental and applied perspective, for the construction of surface molecular nanostructures and nanodevices (3-13). A self-organized molecular pattern with control of structure and derived concomitant function could provide promising materials for the construction of nanodevices that cannot be prepared by conventional microfabrication. The arrangement of adsorbed molecules onto a surface depends on both intermolecular and molecule-surface interactions. For example, Hipps and colleagues (3, 4) prepared a self-organized 2D bifunctional structure on a Au (111) Metal-containing macrocycles with high symmetry and precise architecture are a new class of promising supramolecules for future application in nanotechnology because of their exact shape and size, as well as magnetic, photophysical, and electrostatic properties (14)(15)(16)(17)(18)(19)(20)(21)(22)(23)(24)(25)(26)(27). In this article, we describe scanning tunneling microscopy (STM) studies of the self-assembled supramolecular metallacyclic rectangle, cyclobis [(1, ) 2 )anthracene)(1,4Ј-bis(4-ethynylpyridyl)benzene](PF 6 ) 4 , (Fig. 1) (28). The dimensions of a single rectangle molecule were independently determined to be 3.1 nm long by 1.2 nm wide, from the previously reported x-ray crystallographic data (28). The molecular adlayers were prepared on highly oriented pyrolytic graphite (HOPG) and Au(111) surfaces to investigate the effect of substrate on adlayer formation. The molecules self-organize into well ordered 2D adlayers on both surfaces, and high-resolution STM results clearly reveal an intact rectangle on both HOPG and Au (111) surfaces, but the symmetry and molecular orientation the molecules adopt depends on the substrate. Materials and MethodsChemicals. The PF 6 Ϫ salt of the rectangle was prepared analogously to the ClO 4 Ϫ salt previously reported (28), substituting KPF 6 for NaClO 4 .Substrates. HOPG (quality ZYB) was purchased from Digital Instruments (Santa Barbar...

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Metal Ion Complexation: A Route to 2 D Templates?

Cited by 64 publications

References 57 publications

Two-dimensional assembly and local redox-activity of molecular hybrid structures in an electrochemical environment

Two-dimensional assembly and local redox-activity of molecular hybrid structures in an electrochemical environment

Water-induced correlation between single ions imaged at the solid–liquid interface

Mesoscopic self-organization of a self-assembled supramolecular rectangle on highly oriented pyrolytic graphite and Au(111) surfaces

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