Influence of External Stress on Surface Reaction Dynamics

Uesugi-Saitow, Yuki; Yata, Masanori

doi:10.1103/physrevlett.88.256104

Cited by 34 publications

(15 citation statements)

References 27 publications

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“…It has been revealed on the basis of the first-principles calculations that the lattice strain influences various phenomena at the surfaces such as the growth mode of metal thin films 1,2 and catalytic reactions. [3][4][5][6] The latter, that is, the chemical reaction changes induced by strain on the surfaces, has been studied experimentally by using scanning tunneling microscopy ͑STM͒, 3,7,8 molecular beams, 9,10 and reflection absorption infrared spectroscopy. 11 While these changes originate from that of the electronic structure at the surface, little effort has been devoted to confirming it experimentally so far.…”

Section: Introductionmentioning

confidence: 99%

Strain-induced change in electronic structure of Cu(100)

et al. 2007

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We have studied the electronic structure change of the Cu͑100͒ surface due to the lattice strain both experimentally and theoretically. In the experiments, the surface lattice is compressed by partial nitrogen adsorption. Detailed measurements were made using angle-resolved photoemission spectroscopy with synchrotron and He I radiations. We mainly focused on surface states at the d-band top and bottom, and also sp states ͑Shockley state͒ at X . The d-band bottom shifts toward higher binding energy, while the d-band top shifts toward the Fermi level. This is the direct evidence experimentally indicating the d-band broadening due to the lattice-constant reduction. The observation of the shift of the Shockley state beyond the Fermi level indicates the large electronic redistribution in the sp band. The changes in the electronic structures in the experiments are in good agreement with the results by first-principles calculations. The directions of the energy shifts due to the lattice contraction are well understood by considering the symmetry of the corresponding wave functions at each point of the surface Brillouin zone. An increase of the work function due to the lattice contraction is also discussed in terms of the first-principles calculations. This also implies the special redistribution of Cu 4sp electrons, which can significantly influence the chemical reaction on noble metals. Finally, the lattice-constant reduction is quantitatively estimated from the folding point shift of a surface state at the Brillouin-zone boundary.

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Section: Introductionmentioning

confidence: 99%

Strain-induced change in electronic structure of Cu(100)

et al. 2007

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“…For instance, metal layers epitaxially grown onto single-crystal metal substrates with different lattice constants have been proposed as very efficient selective catalysts in reactions involving H 2 molecules [4]. This is a consequence of the well established fact that modifying the lateral lattice constant of a surface by introducing strain can strongly influence its reactivity [5][6][7][8][9][10].…”

Section: Introductionmentioning

confidence: 99%

Initial Sticking Coefficient of H2 on the Pd–Cu(111) Surface Alloy at very Low Coverages

Farı́as

Minniti

Taleb

et al. 2013

Zeitschrift Für Physikalische Chemie

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Surface Alloys / Hydrogen Dissociation / ReactivityWe present an experimental study of the initial dissociative sticking probability of H 2 on the PdCu(111) surface alloy at Pd coverages between 1-10%. The measurements have been performed using a supersonic molecular beam with an incident energy range E i = 75-163 meV. In agreement with a recent STM study, our results confirm that small amounts of Pd atoms significantly increase the reactivity of the inert Cu(111) surface, although the measured initial sticking probability values were found to be much lower than the ones estimated from the STM work. For a Pd coverage of 1% and E i ∼ 0.10 eV, the H 2 initial sticking probability was found to be 2 × 10 −3 , increasing to 4 × 10 −3 for a Pd coverage of 10%. This agrees well with a recent molecular dynamics study, in which the initial sticking probability was estimated in 7 × 10 −3 for a Pd coverage of 11% and E i ∼ 0.15-0.20 eV. Essentially the same values were measured in the whole incident energy range investigated. Therefore, our results support the main conclusion of the molecular dynamics calculations about the mechanism leading to the increase of reactivity of the Pd-Cu(111) surface alloy, which combines a lower activation energy barrier for dissociation of ∼ 0.25 eV on top of substitutional Pd atoms with spillover onto the Cu(111) surface.

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“…The dissociative sticking coefficient of O 2 was also enhanced for a mechanically stretched Cu single crystal. [8] However, strain achieved by this method was very limited because plastic deformations had to be avoided, and the dissociative sticking coefficient varied by only approximately 10 %. To play a role in catalysis, strain must be large, which is probably the case only in the immediate neighborhood of defects.…”

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confidence: 99%