Energy dissipation during desorption of reaction products: the role of substrate phonons

Gumhalter, B.; Matsushima, Toshiyasu

doi:10.1016/j.susc.2004.05.009

Cited by 13 publications

(6 citation statements)

References 78 publications

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“…A profound knowledge of the atomic vibrational properties of nanostructured materials is of great fundamental and technological importance since the vibrational properties, in particular the vibrational density of states (VDOS), are the key to an understanding of thermodynamic properties like heat capacity, vibrational entropy, mean sound velocity, Debye temperature, and thermal conductivity, as well as electron-phonon coupling and 1/f noise of electronic devices [1][2][3][4]. Moreover, phonon-assisted chemical reactions might play an important role in some catalytic properties of nanoclusters [5].…”

Section: Introductionmentioning

confidence: 99%

Atomic vibrations in iron nanoclusters: Nuclear resonant inelastic x-ray scattering and molecular dynamics simulations

et al. 2007

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The lattice vibrational dynamics of supported, self-assembled, isolated 57 Fe nanoclusters was studied by nuclear resonant inelastic X-ray scattering and molecular dynamics calculations. The morphological and structural properties and the chemical state of the experimental nanoclusters were investigated by atomic force microscopy, high resolution transmission electron microscopy and X-ray photoelectron spectroscopy. The measured and calculated vibrational density of states (VDOS) reveal an enhancement of the low-and high-energy phonon modes and provide experimental and theoretical proof of non-Debye-like behavior in the low-energy region of the VDOS. Experimentally, this effect was found to depend on the nature of the surface shell (oxide or carbide) of the core/shell nanoclusters. According to the calculations for supported isolated pure Fe nanoclusters, the non-Debye-like behavior appears not only in the surface shell, but also in the bcc-Fe core of the nanocluster due to the hybridization of surface and bulk modes.

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Section: Introductionmentioning

confidence: 99%

Atomic vibrations in iron nanoclusters: Nuclear resonant inelastic x-ray scattering and molecular dynamics simulations

et al. 2007

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“…Furthermore, little is known about energy transfer between surfaces and desorbing molecules. Significant energy transfer was already predicted for reactive CO 2 desorption 47. The angular distribution of internally excited molecules might show distributions different from those of the ground state molecules.…”

Section: Discussionmentioning

confidence: 87%

Spatial distributions of desorbing products in basic catalytic processes and surface nano‐structures

Matsushima

Rzeznicka

2005

The Chemical Record

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Reviews of recent progress in angle-resolved measurements of desorbing surface reaction products are discussed. The angular and velocity distributions of desorbing products deliver information about the reaction site as well as the reaction mechanism when the products are repulsively desorbed. These distribution measurements can yield symmetry and orientation information of the reaction site for associative processes whereas, in dissociative desorption, the collimation of fragment desorption is related to the orientation of the intermediate species immediately before dissociation. These different collimations provide information on desorption steps whenever any step becomes rate determining.

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“…This is related to the exothermic reaction heat, which can be distributed to translational and internal (vibrational and rotational) energies of desorbed molecules, and it can also be distributed to the surface. 27,38 It is thought that the energy distribution to the surface can become lower at the higher surface temperatures. 25 On the other hand, the T V AV value on Pt(110) increases with decreasing T S at low temperatures of 625-700 K, indicating that the vibrational states of the desorbed CO 2 are changed at around 700 K on Pt(110).…”

Section: Resultsmentioning

confidence: 99%

IR Chemiluminescence Probe of the Vibrational Energy Distribution of CO₂ Formed during Steady-State CO Oxidation on Pt(111) and Pt(110) Surfaces

et al. 2005

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The infrared (IR) chemiluminescence spectra of CO2 were measured during the steady-state CO + O2 reaction over Pt(110) and Pt(111) surfaces. Analysis of the IR emission spectra indicates that the bending vibrational temperature (TVB), as well as the antisymmetric vibrational temperature (TVAS), was higher on Pt(110) than on Pt(111). On the Pt(110) surface, the highly excited bending vibrational mode compared to the antisymmetric vibrational mode was observed under reaction conditions at low CO coverage (theta(CO) < 0.2) or at high surface temperatures (TS > or = 700 K). This can be related to the activated complex of CO2 formation in a more bent form on the inclined (111) terraces of the Pt(110)(1 x 2) structure. On the other hand, at high CO coverage (theta(CO) > 0.2) or at low surface temperatures (TS < 650 K), TVAS was higher than TVB, which can be caused by the reconstruction of the Pt(110)(1 x 2) surface to the (1 x 1) form with high CO coverage.

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Energy dissipation during desorption of reaction products: the role of substrate phonons

Cited by 13 publications

References 78 publications

Atomic vibrations in iron nanoclusters: Nuclear resonant inelastic x-ray scattering and molecular dynamics simulations

Atomic vibrations in iron nanoclusters: Nuclear resonant inelastic x-ray scattering and molecular dynamics simulations

Spatial distributions of desorbing products in basic catalytic processes and surface nano‐structures

IR Chemiluminescence Probe of the Vibrational Energy Distribution of CO₂ Formed during Steady-State CO Oxidation on Pt(111) and Pt(110) Surfaces

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Energy dissipation during desorption of reaction products: the role of substrate phonons

Cited by 13 publications

References 78 publications

Atomic vibrations in iron nanoclusters: Nuclear resonant inelastic x-ray scattering and molecular dynamics simulations

Atomic vibrations in iron nanoclusters: Nuclear resonant inelastic x-ray scattering and molecular dynamics simulations

Spatial distributions of desorbing products in basic catalytic processes and surface nano‐structures

IR Chemiluminescence Probe of the Vibrational Energy Distribution of CO2 Formed during Steady-State CO Oxidation on Pt(111) and Pt(110) Surfaces

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Product

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IR Chemiluminescence Probe of the Vibrational Energy Distribution of CO₂ Formed during Steady-State CO Oxidation on Pt(111) and Pt(110) Surfaces