Potential energy of hydrogen atom motion on Pd(111) surface and in subsurface: A first principles calculation

Ozawa, Nobuki; Roman, Tanglaw; Nakanishi, Hiroshi; Kasai, Hideaki; Arboleda, Nelson B.; Diño, Wilson Agerico

doi:10.1063/1.2749295

Cited by 50 publications

(35 citation statements)

References 35 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The lesser saturated ridge-Pd atoms also justifies the calculated stronger binding energy in comparison to the pseudo-threefold site of unreconstructed Pd(1 1 0) and even with the reported binding energy of H on fcc site ($0.50 eV) of Pd(1 1 1) [27,33]. Notably, the adsorption site of H on the missing-row surface is the fcc hollow site which rationalizes the obtained configuration presented in Fig.…”

Section: Resultssupporting

confidence: 86%

“…The projector augmented wave (PAW) method [26] is utilized to describe the ionic cores and the Kohn-Sham one-electron valence states are expanded in a basis of plane waves with an energy cutoff of 400 eV. The obtained equilibrium lattice constant of bulk Pd system is 3.94 Å which is in good agreement with results from previous works [27,28].…”

Section: Computational Detailssupporting

confidence: 80%

See 1 more Smart Citation

Understanding the mechanism of H atom absorption in the Pd(1 1 0) surface

Padama

Kasai

2015

Journal of Alloys and Compounds

Self Cite

View full text Add to dashboard Cite

a b s t r a c tThe underlying mechanism of H atom absorption in the Pd(1 1 0) (1 Â 2) missing-row reconstructed surface is investigated by performing density functional theory based calculations. The stronger binding energy of H on ridge than on trough site of the missing-row surface is due to the more pronounced creation of derived bonding state as had been depicted from the electronic structure of the system. Hydrogen absorption takes place with the involvement of other incoming H atoms through an assisted absorption process that is facilitated by the repulsion between the incoming H and the absorbing H. The geometry of the missing-row surface enables the Pd atoms to accommodate the H atoms efficiently leading to H absorption as well as H 2 dissociation.

show abstract

Section: Resultssupporting

confidence: 86%

Section: Computational Detailssupporting

confidence: 80%

Understanding the mechanism of H atom absorption in the Pd(1 1 0) surface

Padama

Kasai

2015

Journal of Alloys and Compounds

Self Cite

View full text Add to dashboard Cite

show abstract

“…For more details, the reader is referred to our previous work. 23 We use the potential energy surface of Osawa et al 30 to describe the interaction of the hydrogen atom with the surface. The Osawa surface was obtained from periodic DFT calculations, similar to ours as reported below.…”

Section: Anharmonic Subsystem Eigenstatesmentioning

confidence: 99%

Electronic damping of anharmonic adsorbate vibrations at metallic surfaces

2010

View full text Add to dashboard Cite

The nonadiabatic coupling of an adsorbate close to a metallic surface leads to electronic damping of adsorbate vibrations and line broadening in vibrational spectroscopy. Here, a perturbative treatment of the electronic contribution to the lifetime broadening serves as a building block for a new approach, in which anharmonic vibrational transition rates are calculated from a position-dependent coupling function. Different models for the coupling function will be tested, all related to embedding theory. The first two are models based on a scattering approach with ͑i͒ a jellium-type and ͑ii͒ a density functional theory based embedding density, respectively. In a third variant a further refined model is used for the embedding density, and a semiempirical approach is taken in which a scaling factor is chosen to match harmonic, single-site, first-principles transition rates, obtained from periodic density functional theory. For the example of hydrogen atoms on ͑adsorption͒ and below ͑subsurface absorption͒ a Pd͑111͒ surface, lifetimes of and transition rates between vibrational levels are computed. The transition rates emerging from different models serve as input for the selective subsurface adsorption of hydrogen in palladium starting from an adsorption site, by using sequences of infrared laser pulses in a laser distillation scheme.

show abstract

“…25,26 The barrier to resurfacing for the rigid clean surface (273 meV) is somewhat higher than that of previous calculations (198 meV). 27 The discrepancies could be due to the choice of pseudopotentials and other convergence parameters. In particular, the sampling of the Brillouin zone is here much higher (8 Â 8 Â 1 vs. 4 Â 4 Â 1), whereas the energy cutoff for the plane wave basis is much lower (340.1 eV vs. 816.34 eV).…”

Section: Model Systemmentioning

confidence: 99%

Manipulating interfacial hydrogens at palladium via STM

Tremblay

Blanco-Rey

2015

Phys. Chem. Chem. Phys.

View full text Add to dashboard Cite

In this contribution, we provide a detailed dynamical analysis of the interfacial hydrogen migration mediated by scanning tunneling microscopy (STM). Contributions from the STM-current and from the non-adiabatic couplings are taken into account using only first principle models. The slight asymmetry of the tunnelling rates with respect to the potential bias sign inferred from experimental observations is reproduced by weighting the contributions of the metal acceptor-donor states for the propagation of the impinging electrons. The quasi-thermal inelastic collision mechanism is treated perturbatively. The influence of hydrogen pre-coverage is also investigated using new potential energy surfaces obtained from periodic density functional theory calculations. Fully quantum dynamical simulations of the system evolution are performed by solving the Pauli master equation, providing insight into the reaction mechanism of STM manipulation of subsurface hydrogens. It is observed that the hydrogen impurity favors resurfacing over occupation of the bulk and subsurface sites whenever possible. The present simulations give strong indication that the experimentally observed protuberances after STM-excitation are due to hydrogen accumulating in the vicinity of the surface.

show abstract

Potential energy of hydrogen atom motion on Pd(111) surface and in subsurface: A first principles calculation

Cited by 50 publications

References 35 publications

Understanding the mechanism of H atom absorption in the Pd(1 1 0) surface

Understanding the mechanism of H atom absorption in the Pd(1 1 0) surface

Electronic damping of anharmonic adsorbate vibrations at metallic surfaces

Manipulating interfacial hydrogens at palladium via STM

Contact Info

Product

Resources

About