Anomalous Potential Dependence in Homoepitaxial Cu(001) Electrodeposition: An<i>In Situ</i>Surface X-Ray Diffraction Study

Golks, Frederik; Stettner, J.; Gründer, Yvonne; Krug, Klaus; Zegenhagen, J.; Magnussen, Olaf M.

doi:10.1103/physrevlett.108.256101

Cited by 26 publications

(28 citation statements)

References 21 publications

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“…[5,6] in situ scanning tunneling microscopy (STM) studies have shown that halides enhance the coarsening of nanoscale islands and pits on Au and Cu electrodes [7][8][9] and affect the structure and dynamics of atomic steps on the metal surface. [18,19] These phenomena have been linked to the structural and redox properties of the metal-halide complexes and the halide adlayer, but detailed microscopic insights into the role of halides on the interface dynamics are still largely missing. [18,19] These phenomena have been linked to the structural and redox properties of the metal-halide complexes and the halide adlayer, but detailed microscopic insights into the role of halides on the interface dynamics are still largely missing.…”

Section: Introductionmentioning

confidence: 99%

Sulfide Surface Dynamics on Cu(100) and Ag(100) Electrodes in the Presence of c(2×2) Halide Adlayers

Rahn

Magnussen

2018

ChemElectroChem

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The influence of coadsorbed anions on electrode surface dynamics is studied in situ by direct observation of single adsorbed species via high-speed scanning tunneling microscopy. Using well-defined model systems, sulfide adsorbates on Cu(100) and Ag(100) covered by c(2 2) ordered adlayers of chloride or bromide, the influence of halide coadsorbate and the metal substrate on the dynamic behavior is systematically evaluated and quantitatively analyzed. The sulfide tracer diffusion coefficients exhibit a pronounced exponential potential dependence in all systems, caused by the effect of the double layer's electric field on the diffusion barrier. The sulfide mobility in general decreases with potential, with the surprising exemption of the Br-covered Cu(100) surface where it increases, indicating a different transport mechanism. In contrast to this strong influence of the halide species on the surface diffusion, the sulfide-sulfide interactions seem to be less affected by the nature of the coadsorbate, but depend more strongly on the type of metal substrate. In addition, the dynamic behavior of clusters on the surface, the formation of grooves, caused by adsorbate-induced vacancy generation, and the adlayer structure and dynamics at high sulfide coverage is discussed for bromide-covered surfaces. The data indicate a tendency of bromide to enhance the transfer of sulfide adsorbates to sites within the metal surface layer.

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Section: Introductionmentioning

confidence: 99%

Sulfide Surface Dynamics on Cu(100) and Ag(100) Electrodes in the Presence of c(2×2) Halide Adlayers

Rahn

Magnussen

2018

ChemElectroChem

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“…7,8,[54][55][56][57][58][59] These investigations provide unparalleled insight into single crystal homoepitaxial growth at the solid-liquid interface, which can deviate significantly from features observed in systems operated under ultra-high vacuum. 60 The homoepitaxial system was used to validate the results in this paper against previously published surface nucleation and growth calculations.…”

Section: Resultsmentioning

confidence: 99%

Numerical Scaling Studies of Kinetically-Limited Electrochemical Nucleation and Growth with Accelerated Stochastic Simulations

Bezzola

Bales

Petzold

et al. 2014

J. Electrochem. Soc.

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A stochastic atomic-scale lattice-based numerical method based on the Exact Lattice First Passage Time method was developed for the simulation of the early stages of kinetically controlled electrochemical nucleation and growth. Electrochemical reaction and surface diffusion on a hexagonal lattice was accounted for in a pristine physical model system that included edge diffusion along steps, and movement over step edges with Ehrlich-Schwöbel barrier. Five cases were investigated: homoexpitaxy, heteroepitaxy, multi-layer growth, terraces, and confined regions. For each, the influence of the physical parameters, deposition conditions, and system geometry on growth morphology was investigated. Simulation based studies of multilayer surface morphology were able to distinguish between layer-by-layer and island growth modes. On stepped terraces, parameter regions associated with he surface diffusion to deposition flux ratio (D/F) and the Ehrlich-Schwöbel barrier were identified under which deposition occurred either at the step edge or by nucleation and growth of islands on the terraces. The probability of growing single crystals in a small confined region was found to scale with D/F and the radius squared.

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“…Excluding applications of qXRR, there are two ways in the literature that timeresolved XRR measurements are typically performed: either by performing Parratt reflectivity scans with low time resolution on processes that are sufficiently slow or that can be halted (Sinsheimer et al, 2013;Lee et al, 2014;Devloo-Casier et al, 2014) or by recording the intensity at one q z -point as a function of time, typically near the anti-Bragg (Nahm & Engstrom, 2016;Golks et al, 2012;Fleet et al, 2005). We show two sets of qXRR data that are analogous to each of these methods.…”

Section: Time-resolved Heteroepitaxymentioning

confidence: 99%

Quick X-ray reflectivity using monochromatic synchrotron radiation for time-resolved applications

Joress

Brock

Woll

2018

J Synchrotron Radiat

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We describe and demonstrate a new technique for parallel collection of x-ray reflectivity data, compatible with monochromatic synchrotron radiation and flat substrates, and apply it to the in-situ observation of thin-film growth. The method employs a polycapillary x-ray optic to produce a converging fan of radiation, incident onto a sample surface, and an area detector to simultaneously collect the XRR signal over an angular range matching that of the incident fan. Factors determining the range and instrumental resolution of the technique in reciprocal space, in addition to the signalto-background ratio, are described in detail. Our particular implementation records is the first method that is both sample-independent and compatible with the highly collimated, monochromatic radiation typical of 3rd generation synchrotron sources.Further, our technique can be readily adapted for use with laboratory-based sources.

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Anomalous Potential Dependence in Homoepitaxial Cu(001) Electrodeposition: AnIn SituSurface X-Ray Diffraction Study

Cited by 26 publications

References 21 publications

Sulfide Surface Dynamics on Cu(100) and Ag(100) Electrodes in the Presence of c(2×2) Halide Adlayers

Sulfide Surface Dynamics on Cu(100) and Ag(100) Electrodes in the Presence of c(2×2) Halide Adlayers

Numerical Scaling Studies of Kinetically-Limited Electrochemical Nucleation and Growth with Accelerated Stochastic Simulations

Quick X-ray reflectivity using monochromatic synchrotron radiation for time-resolved applications

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