Monitoring the Transitions of the Charge-Induced Reconstruction of Au(110) by Reflectance Anisotropy Spectroscopy

Mazine, V.; Borensztein, Y.

doi:10.1103/physrevlett.88.147403

Cited by 53 publications

(72 citation statements)

References 25 publications

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“…Mazine and Borensztein [53,54] find the intensity of the feature observed at 2.6 eV in the spectrum to increase as the potential is made more positive. In our earlier study we observed the intensity of this feature to be reduced as the potential was made more positive [52].…”

Section: Discussionmentioning

confidence: 95%

“…This difference in the dependence of the spectra on the value of the applied potential lead the two groups to make an opposite assignment of RA spectral profiles to the Au(110) (1 × 2) and (1 × 1) reconstructions since the voltage dependence of the transition between these reconstructions has been established from STM studies [66]. This issue has been discussed [52][53][54][55] and reviewed recently [47] and it is clear that an unambiguous identification of RA spectra with surface reconstructions at Au(110) electrodes in an electrochemical cell has not yet been established. It is likely that the differences observed in the RA spectra arise from differences in the morphology of the Au(110) surfaces.…”

Section: Discussionmentioning

confidence: 95%

“…Recently, RA spectra of flame annealed Au(110) surfaces forming the working electrode of an electrochemical cell have been obtained by two groups [52][53][54][55] and the results compared with those ob-tained from clean Au(110) (1 × 2) surfaces prepared in ultra high vacuum (UHV) [52,[56][57][58][59][60]. These studies demonstrate the potential of RAS as an in-situ probe of electrochemical processes.…”

Section: Introductionmentioning

confidence: 94%

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A reflectance anisotropy spectroscopy study of underpotential deposition of copper onto Au(110)

Farell

Lucas

et al. 2005

Physica Status Solidi (b)

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The underpotential deposition of Cu on Au(110) has been monitored by Reflection Anisotropy Spectroscopy (RAS). The changes in the intensity of spectral features observed at 2.6 eV and 3.4 eV in the RA spectrum of Au (110) that are induced by the deposition of Cu occur on different timescales. It is suggested that these changes arise, respectively, from the partial quenching of surface states and from changes in surface morphology.

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Section: Discussionmentioning

confidence: 95%

Section: Discussionmentioning

confidence: 95%

Section: Introductionmentioning

confidence: 94%

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A reflectance anisotropy spectroscopy study of underpotential deposition of copper onto Au(110)

Farell

Lucas

et al. 2005

Physica Status Solidi (b)

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“…Detailed investigations regarding this phenomenon for metal/solution interfaces [2] were performed by employing various ex-situ techniques [3,4] such as low-energy electron diffraction (LEED), reflection high-energy electron diffraction (RHEED), and structure-sensitive techniques such as in-situ scanning tunneling microscopy (STM) [5], in-situ X-ray diffraction (XRD) [6] and reflection anisotropy spectroscopy [7]. While studying reconstructed surfaces in an electrochemical environment, it was found that at electrode potentials positive of the potential of zero charge (E pzc ), the reconstruction is lifted and the surface morphology changes to the bulk-truncated structure [2,8].…”

Section: Introductionmentioning

confidence: 99%

First principles studies of the potential-induced lifting of the Au(100) surface reconstruction

Venkatachalam

Kaghazchi

Kibler

et al. 2008

Chemical Physics Letters

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The potential-induced surface reconstruction of Au(100) has been studied by a combination of density functional theory and thermodynamic considerations. Surface free energies of reconstructed-(5×1) and unreconstructed-(1×1) surfaces were calculated as function of an external electric field using the extended ab-initio atomistic thermodynamics approach. After relating electric field and electrode potential by using capacitance measurements, we calculate lifting of the reconstruction to occur at 0.58 V in 0.01 M HClO 4 and 0.27 V in 0.01 M H 2 SO 4 , being in agreement with the experimental values of 0.60 V and 0.27 V (vs. SCE). Finally, the consequences of using experimental capacitance measurements for calculating surface free energies are discussed.

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“…The ETF 2e is inaccessible on reducing the engineered protein chemically as observed for a wild-type protein [9]. However, the reduction of ETF to the 2-electron reduced species is achievable by electrochemical methods [19]. Protein (63 μM) was contained in 50 mM potassium phosphate buffer, pH 7.0 at 25 °C and maintained under anaerobic conditions.…”

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confidence: 99%

Evidence for protein conformational change at a Au(110)/protein interface

Messiha

Scrutton

et al. 2008

Europhys. Lett.

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Evidence is presented that reflection anisotropy spectroscopy (RAS) can provide real-time measurements of conformational change in proteins induced by electron transfer reactions. A bacterial electron transferring flavoprotein (ETF) has been modified so as to adsorb on an Au(110) electrode and enable reversible electron transfer to the protein cofactor in the absence of mediators. Reversible changes are observed in the RAS of this protein that are interpreted as arising from conformational changes accompanying the transfer of electrons.While there has been considerable progress in the determination of the structures of biological molecules using techniques like X-ray diffraction, there has been very little progress in obtaining information on the time-dependent conformational changes that are the key to understanding the function of such molecules. The importance of extensive motion of protein domains coupled to biological electron transfer has come to light in recent years, primarily through structural analysis of redox proteins using crystallographic methods [1,2]. Domain motion shortens electron tunneling distances through conformational search mechanisms, thus increasing the probability of electron transfer by quantum-mechanical tunneling [3]. Despite these advances, real-time observation of conformational change coupled to electron transfer is difficult and we lack a method of directly probing conformational change linked to redox chemistry in real time that is generally applicable to biological macromolecules. In this work we show that the introduction of surface-exposed cysteine groups into proteins can lead to the creation of protein-Au(110) assemblies suitable for combined electrochemical and reflectance anisotropy spectroscopy (RAS) studies of conformational changes driven by electron transfer. We report real-time measurements of changes in RA spectra that are correlated with the changes in electrode potential. In natural systems such changes in electrode potential induce electron transfer interactions that lead to changes in the conformation of protein domains.The experiments were performed on the electron transfer flavoproteins (ETFs) that act as carriers of electrons between a number of donor and acceptor proteins [4]. They are dynamic molecules both in complex with donor proteins [1,2] and free in solution [5,6]. They have a 2-electron reduction capacity, but thermodynamically are restricted to 1-electron reduction/ oxidation in biological cells. The crystallographic structure of human and bacterial ETFs are known [1,7], thus facilitating a knowledge-based design of surface-exposed cysteine groups. Prior to the RAS experiments the mid-point reduction potential of the FAD cofactor in the engineered ETF proteins was determined as described previously for a wild-type ETF [9]. Enzyme solutions were electrochemically titrated using sodium dithionite as reductant and potassium ferricyanide as oxidant. The UV-visible spectra of ∼30 to 40 points from 300 to 800 nm (4.1 to 1.6 eV) across a whole ran...

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Monitoring the Transitions of the Charge-Induced Reconstruction of Au(110) by Reflectance Anisotropy Spectroscopy

Cited by 53 publications

References 25 publications

A reflectance anisotropy spectroscopy study of underpotential deposition of copper onto Au(110)

A reflectance anisotropy spectroscopy study of underpotential deposition of copper onto Au(110)

First principles studies of the potential-induced lifting of the Au(100) surface reconstruction

Evidence for protein conformational change at a Au(110)/protein interface

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