Oxygen Abstraction from Dioxygen on the Al(111) Surface

Komrowski, Andrew J.; Sexton, Jonathan Z.; Kummel, Andrew C.; Binetti, Marcello; Weiße, Olaf; Hasselbrink, Eckart

doi:10.1103/physrevlett.87.246103

Cited by 108 publications

(86 citation statements)

References 38 publications

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“…[77] The dynamics of O2 adsorption on Al(111) remained unclear despite many years of research. [40] They clarified that O2 reacts with its axis nearly parallel to the surface at kinetic energies of less than 0.2 eV. Their results elucidated that the abstraction process, which occurs when the O2 axis is perpendicular to the surface, is a minor event at low-energy conditions.…”

Section: Molecular Orientation Effectsmentioning

confidence: 91%

“…The dynamics of O2 molecules on the surface in the hyperthermal energy region were also studied in detail on metal and semiconductor surfaces. [40,[48][49][50][51][52][53] In the hyperthermal energy region, we also expect the efficient collision-induced processes proposed by Ceyer. [47] Collisioninduced absorption (CIA) [43,54] and local heating of the substrate [55] were indeed shown to be effective for inducing oxide nucleation, opening up new possibilities for the production of nanostructured metal oxides.…”

Section: Translational Energy Effectsmentioning

confidence: 97%

“…Translationalenergy-induced effects in gas-surface reactions have been studied extensively in terms of gas-surface chemical reactions, [4,[40][41][42][43][44][45][46][47][48][49][50][51][52][53] thin-film growth, [42] and so on. When adsorption is translationally activated, hyperthermal molecular beams allow us to simulate the fate of molecules populating the highenergy tail of the Boltzmann distribution.…”

Section: Translational Energy Effectsmentioning

confidence: 99%

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Supersonic Molecular Beam Experiments on Surface Chemical Reactions

Okada

2014

The Chemical Record

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The interaction of a molecule and a surface is important in various fields, and in particular in complex systems like biomaterials and their related chemistry. However, the detailed understanding of the elementary steps in the surface chemistry, for example, stereodynamics, is still insufficient even for simple model systems. In this Personal Account, I review our recent studies of chemical reactions on single-crystalline Cu and Si surfaces induced by hyperthermal oxygen molecular beams and by oriented molecular beams, respectively. Studies of oxide formation on Cu induced by hyperthermal molecular beams demonstrate a significant role of the translational energy of the incident molecules. The use of hyperthermal molecular beams enables us to open up new chemical reaction paths specific for the hyperthermal energy region, and to develop new methods for the fabrication of thin films. On the other hand, oriented molecular beams also demonstrate the possibility of understanding surface chemical reactions in detail by varying the orientation of the incident molecules. The steric effects found on Si surfaces hint at new ways of material fabrication on Si surfaces. Controlling the initial conditions of incoming molecules is a powerful tool for finely monitoring the elementary step of the surface chemical reactions and creating new materials on surfaces.

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Section: Molecular Orientation Effectsmentioning

confidence: 91%

Section: Translational Energy Effectsmentioning

confidence: 97%

Section: Translational Energy Effectsmentioning

confidence: 99%

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Supersonic Molecular Beam Experiments on Surface Chemical Reactions

Okada

2014

The Chemical Record

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“…Examples include vibrationally inelastic scattering of specific diatomic molecules from metal surfaces, 1,16,[27][28][29][30] which may even be accompanied by electron emission, 5 and specific abstraction reactions. 4 Examples of special interest to H-metal interactions include vibrational lifetimes of H-atoms adsorbed to metal surfaces, 31,32 and the direct observation that collisions of H-atoms with metal surfaces may lead to ehp excitation. 3,33 A question that has not yet received a clear answer is how strongly the translational motion of atoms and molecules interacting with metal surfaces is coupled to ehp excitation, for translational energies in the range of chemical interactions.…”

Section: Introductionmentioning

confidence: 99%

Ab initio molecular dynamics calculations on scattering of hyperthermal H atoms from Cu(111) and Au(111)

Kroes

Pavanello

Blanco-Rey

et al. 2014

The Journal of Chemical Physics

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In-plane structure and ordering at liquid sodium surfaces and interfaces from ab initio molecular dynamics J. Chem. Phys. 127, 134703 (2007); 10.1063/1.2781388Publisher's Note: "Ab initio molecular dynamics simulation of the H/InP(100)-water interface" [J. Chem. Phys. 117, 872 (2002) Energy loss from the translational motion of an atom or molecule impinging on a metal surface to the surface may determine whether the incident particle can trap on the surface, and whether it has enough energy left to react with another molecule present at the surface. Although this is relevant to heterogeneous catalysis, the relative extent to which energy loss of hot atoms takes place to phonons or electron-hole pair (ehp) excitation, and its dependence on the system's parameters, remain largely unknown. We address these questions for two systems that present an extreme case of the mass ratio of the incident atom to the surface atom, i.e., H + Cu(111) and H + Au(111), by presenting adiabatic ab initio molecular dynamics (AIMD) predictions of the energy loss and angular distributions for an incidence energy of 5 eV. The results are compared to the results of AIMDEFp calculations modeling energy loss to ehp excitation using an electronic friction ("EF") model applied to the AIMD trajectories, so that the energy loss to the electrons is calculated "post" ("p") the computation of the AIMD trajectory. The AIMD calculations predict average energy losses of 0.38 eV for Cu(111) and 0.13-0.14 eV for Au(111) for H-atoms that scatter from these surfaces without penetrating the surface. These energies closely correspond with energy losses predicted with Baule models, which is suggestive of structure scattering. The predicted adiabatic integral energy loss spectra (integrated over all final scattering angles) all display a lowest energy peak at an energy corresponding to approximately 80% of the average adiabatic energy loss for non-penetrative scattering. In the adiabatic limit, this suggests a way of determining the approximate average energy loss of non-penetratively scattered H-atoms from the integral energy loss spectrum of all scattered H-atoms. The AIMDEFp calculations predict that in each case the lowest energy loss peak should show additional energy loss in the range 0.2-0.3 eV due to ehp excitation, which should be possible to observe. The average non-adiabatic energy losses for non-penetrative scattering exceed the adiabatic losses to phonons by 0.9-1.0 eV. This suggests that for scattering of hyperthermal H-atoms from coinage metals the dominant energy dissipation channel should be to ehp excitation. These predictions can be tested by experiments that combine techniques for generating H-atom beams that are well resolved in translational energy and for detecting the scattered atoms with high energy-resolution. © 2014 AIP Publishing LLC.

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“…This experiment has stimulated novel theoretical studies [8][9][10][11][12]. Moreover, other experiments, such as the dissociative adsorption of O 2 on Al(111) [13][14][15] and the interaction of highly vibrationally excited NO with Cu(111) [16] and Cs covered Au(111) [17] raise the question whether the non-adiabaticity in surface chemical reactions has not been underestimated in the past [18,19]. The size of nonadiabatic effects in the dissociative adsorption or recombinative desorption is lively and controversially discussed [20] referring to systems such as H 2 /Cu(111) [21][22][23][24], N 2 /Ru(001) [22,25,26] and N 2 /W(110) [23].…”

Section: Introductionmentioning

confidence: 99%

Electronic Excitations in the Course of the Reaction of H with Coinage and Noble Metal Surfaces: A Comparison

Schindler

Diesing

Hasselbrink

2013

Zeitschrift für Physikalische Chemie

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The creation of electronic excitations during the reaction of atomic hydrogen on and with coinage and noble metals has been studied using metal-insulator-metal heterostructures. A characteristic current trace is observed when the outer metal surface of the structure is exposed to a 20 s pulse of H atoms. Comparison to the chemical kinetics allows to disentangle the contributions from the different chemical processes to this current. In the case of the coinage metals studied the observation is interpreted to suggest that predominantly electrons excited in connection with the hydrogen recombination reaction are the source of the current. For Pt such phenomenon is not observed. This difference allows insights into the role of the transition state for the non-adiabaticity in this simple chemical reaction.

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Oxygen Abstraction from Dioxygen on the Al(111) Surface

Cited by 108 publications

References 38 publications

Supersonic Molecular Beam Experiments on Surface Chemical Reactions

Supersonic Molecular Beam Experiments on Surface Chemical Reactions

Ab initio molecular dynamics calculations on scattering of hyperthermal H atoms from Cu(111) and Au(111)

Electronic Excitations in the Course of the Reaction of H with Coinage and Noble Metal Surfaces: A Comparison

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