Perspectives for in situ scanning tunnel microscopic imaging of metalloproteins at HOPG surfaces

Andersen, Jens Enevold Thaulov; Jensen, Marianne H.; Møller, Per; Ulstrup, Jens

doi:10.1016/0013-4686(96)00005-9

Cited by 16 publications

(5 citation statements)

References 36 publications

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“…4. We found that the diameter of the highest population of the molecules was 6.5 nm, which is close to the diameter of laccase reported in the literature (5 nm) [43,44]. Small difference may be caused by the tip-broadening effect.…”

Section: Stm Resultssupporting

confidence: 71%

Electroreduction of laccase covalently bound to organothiol monolayers on gold electrodes

Klis

Maicka

Michota

et al. 2007

Electrochimica Acta

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Section: Stm Resultssupporting

confidence: 71%

Electroreduction of laccase covalently bound to organothiol monolayers on gold electrodes

Klis

Maicka

Michota

et al. 2007

Electrochimica Acta

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“…The results of entries 3 and 4 indicate that once the electrode is detached and the H-M configuration is then set again on HV 2+ 2Br - solution the magnitude of the spike response is not fully recovered. The dependence on t m can be due to a change of the surface structure of HOPG, , such as surface process-induced delamination. In fact, as the period passed during which the first H-M configuration was prolonged the vertical width of the cyclic voltammogram in the double-layer potential region became greater, though the characteristics of the spike response itself were unchanged at least in a period of 8 h. Work is currently under way to clarify this time evolution.…”

Section: Resultsmentioning

confidence: 99%

Study of the Voltammetric Spike Response of Heptyl Viologen at a HOPG Electrode Horizontally Touched to a Gas/Heptyl Viologen Aqueous Solution Interface

et al. 2001

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We investigated the electrochemistry of a basal plane highly oriented pyrolytic graphite electrode horizontally touched to a gas/heptyl viologen aqueous solution (G/S) interface using cyclic voltammetry, electroreflectance (ER) spectroscopy, potential step chronoamperometry, chronoreflectometry, and chronocoulometry. The spike response on the voltammogram, which was previously analyzed by Tokuda et al. (see: J. Electroanal. Chem. 1999, 473, 138.), was found to be observable only in restricted conditions. The experimental ER spectrum at the spike potential was in good agreement with the simulated one, indicating that the redox reaction of heptyl viologen takes place at the spike potential and the radical cation adsorbs on the electrode surface in a nonupright orientation. The voltammogram and potential step response suggested that the kinetics of the spike response can be explained in terms of a nucleation-growthcollision (NGC) mechanism. It was revealed that the transient of reflectance in response to the potential step synchronizes with the NGC current component. The plot of the charge as a function of the final potential in the potential step coulometry measurement exhibited a transition point at which the interconversion of the oxidation state amounts to more than half of the adsorbed viologen. The spike response was assigned as the first-order faradaic phase transition, presumably between a Gibbs monolayer and a Langmuir monolayer. The presence of the Gibbs monolayer of heptyl viologen at the G/S interface was confirmed by surface tension measurements.

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“…STM of the redox metalloenzymes laccase (Polypherus Versicolor) 247 and peroxidase (horseradish, HRP) on HOPG 158 have been reported. Only the latter qualifies as in situ STM.…”

Section: Stm Of Redox and Other Metalloproteinsmentioning

confidence: 99%

Electronic Properties of Functional Biomolecules at Metal/Aqueous Solution Interfaces

et al. 2002

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Monolayers of molecules, which retain their function in the adsorbed state on solid surfaces, are important in materials science, analytical detection, and other technology approaching the nanoscale. Molecular monolayers, including layers of functional biological macromolecules, offer new insight in electronic properties and stochastic single-molecule features and can be probed by new methods which approach the single-molecule level. One of these is in situ scanning tunneling microscopy (STM) in which single-molecule electronic properties directly in aqueous solution are probed. In situ STM combined with physical electrochemistry, single-crystal electrodes, and spectroscopic methods is now a new dimension in interfacial bioelectrochemistry. We overview first some approaches to spectroscopic single-molecule imaging, including fluorescence spectroscopy, chemical reaction dynamics, atomic force microscopy, and electrochemical single-electron transfer. We then focus on in situ STM. In addition to high structural resolution, in situ STM offers a single-molecule spectroscopic perspective. This emerges most clearly when adsorbate molecules contain accessible redox levels, and the tunneling current decomposes into successive single-molecule interfacial electron transfer (ET) steps. Theories of electrochemical ET and in situ STM of redox molecules as well as specific cases are addressed. Two-step in situ STM represents different molecular mechanisms and even new ET phenomena, related to coherent many-electron transfer. A number of systems are noted to accord with these views. The discussion is concluded by attention to one of the still very few redox proteins addressed by in situ STM, the blue copper protein Pseudomonas aeruginosa azurin. Use of comprehensive electrochemical techniques has ascertained that well-defined protein monolayers in two opposite orientations can be formed and interfacial tunneling patterns disclosed. P. aeruginosa azurin emerges as by far the most convincing case where in situ STM of functional metalloproteins to single-molecule resolution has been achieved. This comprehensive approach holds promise for broader use of in situ STM as a single-molecule spectroscopy of metalloproteins and illuminates prerequisites and limitations of in situ STM of biological macromolecules.

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Perspectives for in situ scanning tunnel microscopic imaging of metalloproteins at HOPG surfaces

Cited by 16 publications

References 36 publications

Electroreduction of laccase covalently bound to organothiol monolayers on gold electrodes

Electroreduction of laccase covalently bound to organothiol monolayers on gold electrodes

Study of the Voltammetric Spike Response of Heptyl Viologen at a HOPG Electrode Horizontally Touched to a Gas/Heptyl Viologen Aqueous Solution Interface

Electronic Properties of Functional Biomolecules at Metal/Aqueous Solution Interfaces

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