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Electrochemical Characterization of Self-Assembled Monolayers Containing Redox Switching Element
Nováková Lachmanová, Štěpánka ; Kocábová, Jana ; Vavrek, František ; Sebechlebská, Táňa ; Šebera, Jakub ; Kolivoška, Viliam ; Lukášek, J. ; Balzer, N. ; Valášek, M. ; Hromadová, Magdaléna
Adsorption properties of molecules containing [Ru(terpy)2]2+ and [Os(terpy)2]2+ redox switching element connected to the electrode surface by tripodal thiolate anchoring groups have been studied together with their charge transfer properties in the adsorbed form. STM-based current-voltage measurements confirmed that the conductance of self-assembled monolayer containing [Os(terpy)2]2+ redox switching element is lower than that containing [Ru(terpy)2]2+ element. This observation agrees with previously observed differences in the electron transfer rate constants of these molecules in their adsorbed state.
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Electrochemical Characterization of Molecular Conductors Containing Redox Switching Element
Nováková Lachmanová, Štěpánka ; Vavrek, František ; Sebechlebská, Táňa ; Šebera, Jakub ; Kolivoška, Viliam ; Lukášek, J. ; Balzer, N. ; Valášek, M. ; Mayor, M. ; Hromadová, Magdaléna
Electrochemical properties of new molecules containing tripodal anchor and redox switching\nelement have been studied by cyclic voltammetry and DFT quantum mechanical calculations.\nComparison of their redox properties with individual organometallic [Ru(terpy)2]2+t3+ and\n[Os(terpy)2]2+t3+ redox centers shows that covalently bonded tripodal anchor does not\ncompromise the reversibility of a redox process and has no effect on the stability of new\nmolecules. New molecular conductors have smaller HOMO-LUMO gap and both are oxidized\nat only slightly more positive potentials after tripodal substitution making them suitable for the\ndevelopment of molecular conductors with switching abilities.
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Charge Transport through Molecular Towers Based on Tetraphenyhmethane Tripods
Kolivoška, Viliam ; Šebera, Jakub ; Lindner, M. ; Valášek, M. ; Mayor, M. ; Mészáros, G. ; Gasior, Jindřich ; Hromadová, Magdaléna
Molecular platforms with multiple anchors were introduced recently to provide robusi coupling between molecular electronic components and metallic electrodes. In this work, charge transport in tower-shaped single molecule conductors based on tetraphenylmethane tripod possessing three thiol anchors is investigated by scanning tunneling microscopy break junction technique. The effect of tripod substitution pattern and number of repeating units in molecule is addressed. The substitution was found to influence conductance value in early stages of molecular junction evolution, where tower lays parallel to surface. In late stages, the charge is transported through principal molecular axis and junction breaks thermally in tilted configuration.
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Charge Transport in Single Oligophenylene Molecular Wires with Different Anchoring Groups
Hromadová, Magdaléna ; Kolivoška, Viliam ; Šebera, Jakub ; Sebechlebská, Táňa ; Gasior, Jindřich ; Nováková Lachmanová, Štěpánka ; Mészáros, G. ; Lindner, M. ; Mayor, M. ; Valášek, M.
This work compares single molecule conductance measurements of selected organic systems containing identical oligophenylene molecular wires and different tripodal anchoring groups. Single molecule conductance G was obtained by a scanning tunneling microscopy break junction technique complemented by theoretical calculations based on the density functional theory and non-equilibrium Green’s function formalism. Two molecules were compared where the same oligophenylene wire is connected to one of the electrodes via a tripod substituted on each leg by a thiol group either in the meta or para position. By combined experimental and theoretical analysis it was possible to confirm that single molecule conductance in the metal-molecule-metal junction of both molecules corresponds to a fully extended molecular wire, which is attached to one of the electrodes by all three thiolate bonds of the tripod. Experimental results confirmed that G value of meta-connected molecules is lower than that of para, whereas junction formation probability was higher for meta functionalization.
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Charge Transport in Single Oligophenylene Molecular Wires with Different Anchoring Groups
Hromadová, Magdaléna ; Kolivoška, Viliam ; Šebera, Jakub ; Sebechlebská, Táňa ; Gasior, Jindřich ; Nováková Lachmanová, Štěpánka ; Mészáros, G. ; Lindner, M. ; Mayor, M. ; Valášek, M.
This work compares single molecule conductance measurements of selected organic systems containing identical oligophenylene molecular wires and different tripodal anchoring groups. Single molecule conductance G was obtained by a scanning tunneling microscopy break junction technique complemented by theoretical calculations based on the density functional theory and non-equilibrium Green’s function formalism. Two molecules were compared where the same oligophenylene wire is connected to one of the electrodes via a tripod substituted on each leg by a thiol group either in the meta or para position. By combined experimental and theoretical analysis it was possible to confirm that single molecule conductance in the metal-molecule-metal junction of both molecules corresponds to a fully extended molecular wire, which is attached to one of the electrodes by all three thiolate bonds of the tripod. Experimental results confirmed that G value of meta-connected molecules is lower than that of para, whereas junction formation probability was higher for meta functionalization.
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Chronopotentiometry of Papain Modified by Ruthenium Complexes
Nováková Lachmanová, Štěpánka ; Pospíšil, Lubomír ; Talbi, B. ; Salmain, M. ; Hromadová, Magdaléna
Catalytic hydrogen evolution reaction is one of known effects observed during the electrochemical studies of proteins. Constant current chronopotentiometric stripping technique is suitable tool for the study of catalytic hydrogen evolution reaction due to the formation of peak H. This contribution compares the catalytic behaviour of nonmodified papain and its artificial derivatives prepared by the interaction of organometallic complexes of ruthenium with free sulfhydryl group of protein. The comparison of the chronopotentiometric behaviour of papain and its derivatives would help to better understand the catalytic hydrogen evolution reaction in these derivatives.
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Charge Transport in Single Oligophenylene Molecular Wires with Different Anchoring Groups
Hromadová, Magdaléna ; Kolivoška, Viliam ; Šebera, Jakub ; Sebechlebská, Táňa ; Gasior, Jindřich ; Nováková Lachmanová, Štěpánka ; Mészáros, G. ; Lindner, M. ; Mayor, M. ; Valášek, M.
This work compares single molecule conductance measurements of selected organic systems containing identical oligophenylene molecular wires and different tripodal anchoring groups. Single molecule conductance G was obtained by a scanning tunneling microscopy break junction technique complemented by theoretical calculations based on the density functional theory and non-equilibrium Green’s function formalism. Two molecules were compared where the same oligophenylene wire is connected to one of the electrodes via a tripod substituted on each leg by a thiol group either in the meta or para position. By combined experimental and theoretical analysis it was possible to confirm that single molecule conductance in the metal-molecule-metal junction of both molecules corresponds to a fully extended molecular wire, which is attached to one of the electrodes by all three thiolate bonds of the tripod. Experimental results confirmed that G value of meta-connected molecules is lower than that of para, whereas junction formation probability was higher for meta functionalization.
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Influence of Adsorption on Electrochemical Reduction of Pyridinium Derivatives
Nováková Lachmanová, Štěpánka ; Dupeyre, G. ; Lainé, P. P. ; Hromadová, Magdaléna
Two expanded pyridinium-based compounds 1 and 2 were studied by cyclic voltammetry in two different environments. The nonaqueous solution suppresses the adsorption of the compounds on the electrode surface. Adsorption process in aqueous environment was confirmed by typical shape of the curve as well as by the linear dependence of peak current on the scan rate. The shift of standard redox potential in aqueous solution compared to nonaqueous environment toward more negative potential indicates the adsorption of reactant on the electrode surface. Larger shift observed for flat conjugated molecule 1 confirms its stronger adsorption than for the second molecule.
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Determination of Roughness Factor and Fractal Dimension of Zirconium in its Native and Surface Modified State using Atomic Force Microscopy. Effect of the Hydrogen Evolution Reaction on the Surface Structure
Novák, M. ; Kocábová, Jana ; Kolivoška, Viliam ; Pospíšil, Lubomír ; Macák, J. ; Cichoň, Stanislav ; Cháb, Vladimír ; Hromadová, Magdaléna
Atomic force microscopy (AFM) was used to characterize surface morphology of pristine zirconium, Si modified and FeSi modified zirconium electrodes prior and after hydrogen evolution at potentials negative of the open circuit potential value. Two main characteristic parameters were obtained from the ex situ AFM height images, namely, the roughness factor and fractal dimension of the studied surface. The effect of hydrogen evolution reaction on the electrode surface morphology was discussed. Fractal dimension values were used successfully to explain the non ideality of the interfacial capacitance.
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Investigation of Single Molecule Charge Transport Properties and Geometrical Arrangement in Terpyridine Architectures Supported by the Tetraphenylmethane Tripod
Kolivoška, Viliam ; Sebechlebská, Táňa ; Šebera, Jakub ; Gasior, Jindřich ; Lindner, M. ; Lukášek, J. ; Valášek, M. ; Mayor, M. ; Mészáros, G. ; Hromadová, Magdaléna
Tripodal platforms were engineered recently to realize a well-defined directional contact between metallic electrodes and molecular architectures dedicated to serve as working elements for electronic applications. In this work we employ cyclic voltammetry, scanning tunneling microscopy break junction technique and theoretical approaches based on the combination of density functional theory and non-equilibrium Green´s function to investigate the geometrical arrangement and single molecule charge transport in terpyridine-based architectures supported by tetraphenylmethane tripod. We demonstrate that this architecture adopts a favorable geometrical arrangement capable of forming highly conductive molecular junctions and is thus suitable to serve as a basis for working molecular switches.
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