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By studying the tantalum (Ta)(111) surface with X-ray photoemission spectroscopy and density functional theory, we determined binding energy values for the clean Ta(111) (+3.068 eV) and hydrogenated Ta(111) (+3.421 eV) surfaces with an isolated atom level of 18.977 eV. Using the bond–band barrier and zone-selective electron spectroscopy correlation, we investigated the mechanism of hydrogenation adsorption on the Ta(111) surface. We found the local densities of states of the first layer of Ta atoms in the reconstructed structure, which formed on the adsorbent hydrogen of the surface chemical bond contracts and dipole polarization. Moreover, we showed that on the Ta(111) surface, the hydrogen-induced surface core level shifts are dominated by quantum entrapment and are proportional to the calculated hybridized orbitals of the valence band. The latter is therefore correlated to the local surface chemical reactivity and is useful for other adsorbate systems on transition metals. [ABSTRACT FROM AUTHOR]

A combination of photoelectron spectrometric analysis and density functional theory calculations has enabled reconciliation of the bond-energy-electron relaxation for the Ta(100, 110, 111) surfaces chemisorbed with oxygen at different coverages. Results show that increasing oxygen coverage lowers the adsorption energy associated with lattice reconstruction. Valence electrons transfer from Ta surface atoms to oxygen to create four excessive DOS features in terms of O Ta bonding, lone pairs of oxygen, Ta + electron holes, and polarized Ta dipoles. Oxidation proceeds in the following dynamics: oxygen gets electrons from two neighboring Ta atoms left behind Ta + ; the sp 3 -orbital hybridization takes place with additional two electron lone pairs, the lone pairs polarize the other two Ta neighbors becoming dipoles. X-ray photoelectron spectral analysis results in the 4 f binding energy of an isolated Ta atom and its shift upon bond formation and oxidation. Exercises provide not only a promising numerical approach for the quantitative information about the bond and electronic behavior but also consistent insight into the electronic dynamics of metal oxidation. [ABSTRACT FROM AUTHOR]

Abstract: We present an approach for quantifying the heterogeneous interface bond energy using X-ray photoelectron spectroscopy (XPS). Firstly, from analyzing the XPS core-level shift of the elemental surfaces we obtained the energy levels of an isolated atom and their bulk shifts of the constituent elements for reference; then we measured the energy shifts of the specific energy levels upon interface alloy formation. Subtracting the referential spectrum from that collected from the alloy, we can distil the interface effect on the binding energy. Calibrated based on the energy levels and their bulk shifts derived from elemental surfaces, we can derive the bond energy, energy density, atomic cohesive energy, and free energy at the interface region. This approach has enabled us to clarify the dominance of quantum entrapment at CuPd interface and the dominance of polarization at AgPd and BeW interfaces, as the origin of interface energy change. Developed approach not only enhances the power of XPS but also enables the quantification of the interface energy at the atomic scale that has been an issue of long challenge. [Copyright &y& Elsevier]

Abstract: BeW is an important medium for radiation protection in the International Thermonuclear Experimental Reactor (ITER) devices. However, the mechanism for the radiation-protection ability of BeW remains unclear. An extension of the BOLS correlation mechanism into the X-ray photoelectron spectroscopy (XPS) has enabled us to examine the energy and charge distribution of the specimen and clarify that the Be 1s and W 4f7/2 energy levels undergo an elevation by 0.136 and 0.184 times those of the respective bulk constituents standing alone up-on BeW compound formation associated with polarization of the valence density of states. It is suggested that the interface potential barrier creation due to bond order distortion and bond nature alteration perturbs essentially the Hamiltonian and hence leads to the binding energy shifts. The established interface potential barrier and the polarized charge may screen the nuclear irradiation in the thermonuclear fusion devices. Findings may provide guideline for searching materials for such purpose. [ABSTRACT FROM AUTHOR]

Abstract: Materials at heterojunction interfaces demonstrate many physical and chemical properties that are indeed fascinating with mechanisms that need yet to be explored. We show herewith that the “interface charge and energy quantum entrapment due to bond order distortion and bond nature alteration” perturbs essentially the Hamiltonian and hence the binding energy of the CuPd alloy interface. Analyzing the X-ray photoelectron emission of the thermally induced evolution of the Cu 2p and Pd 3d core-level energies at the Cu–Pd interface before and after thermally alloying revealed that the Pd 3d and Cu 2p interfacial potential traps are 0.36 and 0.95 times deeper than the potential wells of the corresponding bulk constituents standing alone. [Copyright &y& Elsevier]

Abstract: An in situ X-ray photoelectron emission investigation revealed that the size trend of the 2p3/2 binding-energy shift (BES) of Ni nanoclusters grown on SiO2 substrate follows the prediction of the bond order–length–strength (BOLS) correlation theory . Theoretical reproduction of the measurements turns out that the 2p3/2 binding energy of an isolated Ni atom is 850.51eV and its intrinsic bulk shift is 2.70eV. Findings confirmed that the skin-depth local strain and potential well quantum trapping induced by the shorter and stronger bonds between under-coordinated surface atoms provide perturbation to the Hamiltonian and hence dominate the size dependent BES. [Copyright &y& Elsevier]