Core electron binding energies of adsorbates on Cu(111) from first-principles calculations

Kahk, Juhan Matthias; Lischner, Johannes

doi:10.1039/c8cp04955f

Cited by 33 publications

(37 citation statements)

References 89 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…In these calculations, a Cu cluster containing 163 Cu atoms, shown in Figure 3, was used to model the Cu(111) surface. The relaxed geometries of the adsorbates on the surface were taken from our previ- ous study [44]. For CO on Cu(111), the "top" adsorption site was used (where the CO sits directly above one of the Cu atoms).…”

Section: Resultsmentioning

confidence: 99%

Accurate absolute core-electron binding energies of molecules, solids, and surfaces from first-principles calculations

Kahk

Lischner

2019

Phys. Rev. Materials

Self Cite

112

View full text Add to dashboard Cite

Core-electron x-ray photoelectron spectroscopy is a powerful technique for studying the electronic structure and chemical composition of molecules, solids and surfaces. However, the interpretation of measured spectra and the assignment of peaks to atoms in specific chemical environments is often challenging. Here, we address this problem and introduce a parameter-free computational approach for calculating absolute core-electron binding energies. In particular, we demonstrate that accurate absolute binding energies can be obtained from the total energy difference of the ground state and a state with an explicit core hole when exchange and correlation effects are described by a recently developed meta-generalized gradient approximation and relativistic effects are included even for light elements. We carry out calculations for molecules, solids and surface species and find excellent agreement with available experimental measurements. For example, we find a mean absolute error of only 0.16 eV for a reference set of 103 molecular core-electron binding energies. The capability to calculate accurate absolute core-electron binding energies will enable new insights into a wide range of chemical surface processes that are studied by x-ray photoelectron spectroscopy. arXiv:1904.04823v1 [cond-mat.mtrl-sci]

show abstract

Section: Resultsmentioning

confidence: 99%

Accurate absolute core-electron binding energies of molecules, solids, and surfaces from first-principles calculations

Kahk

Lischner

2019

Phys. Rev. Materials

Self Cite

112

View full text Add to dashboard Cite

show abstract

“…For all-electron calculations, the problem is more difficult to solve. One approach suggested by Kahk and Lischner [27,107] is to introduce a third step in addition to the ground state and the core-hole calculation. In this intermediate step, the symmetry of the wave function is broken, e.g.…”

Section: The Choice Of Core-hole Localization Methods For Xps Simulat...mentioning

confidence: 99%

The Nuts and Bolts of Ab-Initio Core-Hole Simulations for K-shell X-Ray Photoemission and Absorption Spectra

Klein,

Hall,

Maurer

2020

Preprint

View full text Add to dashboard Cite

X-ray photoemission (XPS) and Near Edge X-ray Absorption Fine Structure (NEXAFS) spectroscopy play an important role in investigating the structure and electronic structure of materials and surfaces. Ab-initio simulations provide crucial support for the interpretation of complex spectra containing overlapping signatures. Approximate core-hole simulation methods based on Density Functional Theory such as the Delta-Self-Consistent-Field (∆SCF) method or the transition potential (TP) method are widely used to predict K-shell XPS and NEXAFS signatures of organic molecules, inorganic materials and metal-organic interfaces at reliable accuracy and affordable computational cost. We present the numerical and technical details of our variants of the ∆SCF and transition potential method (coined ∆IP-TP) to simulate XPS and NEXAFS transitions. Using exemplary molecules in gas-phase, in bulk crystals, and at metal-organic interfaces, we systematically assess how practical simulation choices affect the stability and accuracy of simulations. These include the choice of exchange-correlation functional, basis set, the method of core-hole localization, and the use of periodic boundary conditions. We particularly focus on the choice of aperiodic or periodic description of systems and how spurious charge effects in periodic calculations affect the simulation outcomes. For the benefit of practitioners in the field, we discuss sensible default choices, limitations of the methods, and future prospects.

show abstract

“…The peak at 531.3 eV can be ascribed to the surface O or -OH adsorbed on Cu (1 1 1). The signals at 532.5 and 535.5 eV are corresponding to the physisorbed H 2 O and CO 2 , respectively, on Cu (1 1 1) [55].…”

Section: Synthesis and Structural Characterization Of Cu-n-c Tmentioning

confidence: 99%

Nitrogen-rich metal-organic framework mediated Cu–N–C composite catalysts for the electrochemical reduction of CO2

Cao

Chen

Dong

et al. 2021

Journal of Energy Chemistry

View full text Add to dashboard Cite

Core electron binding energies of adsorbates on Cu(111) from first-principles calculations

Cited by 33 publications

References 89 publications

Accurate absolute core-electron binding energies of molecules, solids, and surfaces from first-principles calculations

Accurate absolute core-electron binding energies of molecules, solids, and surfaces from first-principles calculations

The Nuts and Bolts of Ab-Initio Core-Hole Simulations for K-shell X-Ray Photoemission and Absorption Spectra

Nitrogen-rich metal-organic framework mediated Cu–N–C composite catalysts for the electrochemical reduction of CO2

Contact Info

Product

Resources

About