A first principles investigation of the oxygen adsorption on Zr(0001) surface using cluster expansions

Samin, Adib J.; Taylor, Christopher D.

doi:10.1016/j.apsusc.2017.06.210

Cited by 19 publications

(10 citation statements)

References 45 publications

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“…To test which surface geometries are energetically favourable, heat of formation energies at 0 K, ΔH f (Θ), were calculated as a function of the coverage, Θ, neglecting the pV term and vibrational energies [34,35]:…”

Section: Resultsmentioning

confidence: 99%

Water adsorption on the P-rich GaP(100) surface: optical spectroscopy from first principles

May

Sprik

2018

New J. Phys.

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The contact of water with semiconductors typically changes its surface electronic structure by oxidation or corrosion processes. A detailed knowledge-or even control of-the surface structure is highly desirable, as it impacts the performance of opto-electronic devices from gas-sensing to energy conversion applications. It is also a prerequisite for density functional theory-based modelling of the electronic structure in contact with an electrolyte. The P-rich GaP(100) surface is extraordinary with respect to its contact with gas-phase water, as it undergoes a surface reordering, but does not oxidise. We investigate the underlying changes of the surface in contact with water by means of theoretically derived reflection anisotropy spectroscopy (RAS). A comparison of our results with experiment reveals that a water-induced hydrogen-rich phase on the surface is compatible with the boundary conditions from experiment, reproducing the optical spectra. We discuss potential reaction paths that comprise a water-enhanced hydrogen mobility on the surface. Our results also show that computational RAS-required for the interpretation of experimental signatures-is feasible for GaP in contact with water double layers. Here, RAS is sensitive to surface electric fields, which are an important ingredient of the Helmholtz-layer. This paves the way for future investigations of RAS at the semiconductor-electrolyte interface.

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Section: Resultsmentioning

confidence: 99%

Water adsorption on the P-rich GaP(100) surface: optical spectroscopy from first principles

May

Sprik

2018

New J. Phys.

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“…The resulting structure is similar to a previously reported result, 7 in which adsorption of one ML of water on the (001) surface led to the dissociation of one quarter of the wa- Mixed dissociative adsorption of water on the (001) surface allows for the formation of various To assess stability and likelihood of actual occurrence, we calculated heat of formation energies, Table I for different coverages and different degrees of dissociation. The heat of formation energy as a measure for relative stability is obtained from the total energies, E tot , neglecting the pV term and vibrational energies, 32 as follows:…”

Section: Methodsmentioning

confidence: 99%

Band positions of anatase (001) and (101) surfaces in contact with water from density functional theory

Geiger

Sprik

May

2020

The Journal of Chemical Physics

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Titanium dioxide in the anatase configuration plays an increasingly important role for photo(electro)catalytic applications due to its superior electronic properties when compared to rutile. In aqueous environments, the surface chemistry and energetic band positions upon contact with water determine charge-transfer processes over solid-solid or solid-electrolyte interfaces. Here, we study the interaction of anatase (001) and (101) surfaces with water and the resulting energetic alignment by means of hybrid density functional theory. While the alignment of band positions favours charge-transfer processes between the two facets for the pristine surfaces, we find the magnitude of this underlying driving force to crucially depend on water coverage and degree of dissociation. It can be largely alleviated for intermediate water coverages. Surface states and their passivation by dissociatively adsorbed water play an important role here. Our results suggest that anatase band positions can be controlled over a range of almost one eV via its surface chemistry. File list (2) download file view on ChemRxiv Band_positions_anatase.pdf (4.85 MiB) download file view on ChemRxiv Supplementary_material.pdf (3.53 MiB)

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“…The root mean square error (RMSE) of the fit was 0.032 eV with a leave-one-out cross validation (LOOCV) score of 0.028 eV. In addition, the fit was found to be stable by checking that the histogram of the parameters recorded during the LOOCV procedure followed a normal distribution similar to previous work [68]. Finally, the variation of the binding energy as a function of the local environment is displayed in Figure 1b.…”

Section: Fitting the Cluster Expansion Modelmentioning

confidence: 53%

First-principles localized cluster expansion study of the kinetics of hydrogen diffusion in homogeneous and heterogeneous Fe-Cr alloys

et al. 2019

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Metal alloys have a wide range of technological applications, from structural materials to catalysts. In many situations the transport of hydrogen, whether intentionally for hydrogen storage and fuel cell applications or unintentionally in the case of tritium uptake in nuclear materials, is an important concern. Fe-Cr binary alloys, in particular, may be viewed as a simple model system to represent ferritic steels used in nuclear energy systems and, more generally, as a model binary alloy for examining the role of alloying elements on transport. In this work, we used density functional theory, cluster expansion, and kinetic Monte Carlo to study hydrogen kinetics in Fe-Cr alloys. In random homogenenous alloys, we observed that hydrogen diffusivity first decreased with increasing Cr content and then increased to its levels in pure Cr. Furthermore, the effects of heterogeneity, as might be induced by irradiation, were explored and it was concluded that local structural heterogeneities for the same overall Cr concentration may significantly affect the hydrogen diffusivity. The effect was attributed to the relative binding energy of hydrogen in different metals and this understanding was then utilized to predict hydrogen transport behavior in different element-segregated grain/grain boundary combinations and thus identify solute/solvent alloys where hydrogen transport might be either hindered or

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A first principles investigation of the oxygen adsorption on Zr(0001) surface using cluster expansions

Cited by 19 publications

References 45 publications

Water adsorption on the P-rich GaP(100) surface: optical spectroscopy from first principles

Water adsorption on the P-rich GaP(100) surface: optical spectroscopy from first principles

Band positions of anatase (001) and (101) surfaces in contact with water from density functional theory

First-principles localized cluster expansion study of the kinetics of hydrogen diffusion in homogeneous and heterogeneous Fe-Cr alloys

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