Sticking, adsorption, and absorption of atomic H on Cu(110)

Bischler, U.; Sandl, P.; Bertel, E.; Brunner, T.; Brenig, Wilhelm

doi:10.1103/physrevlett.70.3603

Cited by 66 publications

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“…44 In the case of H/Si, theoretical investigations indicate that the diffusion 19,28,32 and desorption barriers 18 decrease substantially when the Si atoms relax. However, a model involving static lattice distortion of silicon between the two ''hydrogen-adsorbed'' and ''hydrogen-desorbed'' states, and a corresponding barrier change, would lead to a violation of detailed balance.…”

Section: Introductionmentioning

confidence: 99%

Reaction dynamics of molecular hydrogen on silicon surfaces

et al. 1996

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Bratu, P.; Brenig, W.; Gross, A.; Hartmann, M.; Höfer, U.; Kratzer, Peter; Russ, R. Published in:Physical Review B Link to article, DOI:10.1103/PhysRevB.54.5978 Publication date: 1996 Document VersionPublisher's PDF, also known as Version of record Link back to DTU Orbit Citation (APA): Bratu, P., Brenig, W., Gross, A., Hartmann, M., Höfer, U., Kratzer, P., & Russ, R. (1996). Reaction dynamics of molecular hydrogen on silicon surfaces. Physical Review B, 54(8), 5978-5991. DOI: 10.1103/PhysRevB.54.5978 Reaction dynamics of molecular hydrogen on silicon surfaces Experimental and theoretical results on the dynamics of dissociative adsorption and recombinative desorption of hydrogen on silicon are presented. Using optical second-harmonic generation, extremely small sticking probabilities in the range 10 Ϫ9 Ϫ10 Ϫ5 could be measured for H 2 and D 2 on Si͑111͒7ϫ7 and Si͑100͒2ϫ1.Strong phonon-assisted sticking was observed for gases at 300 K and surface temperatures between 550 K and 1050 K. The absolute values as well as the temperature variation of the adsorption and desorption rates show surprisingly little isotope effect, and they differ only little between the two surfaces. These results indicate that tunneling, molecular vibrations, and the structural details of the surface play only a minor role for the adsorption dynamics. Instead, they appear to be governed by the localized H-Si bonding and Si-Si lattice vibrations. Theoretically, an effective five-dimensional model is presented taking lattice distortion, corrugation, and molecular vibrations into account within the framework of coupled-channel calculations. While the temperature dependence of the sticking is dominated by lattice distortion, the main effect of corrugation is a reduction of the preexponential factor by about one order of magnitude per lateral degree of freedom. Molecular vibrations have practically no effect on the adsorption/desorption dynamics itself, but lead to vibrational heating in desorption with a strong isotope effect. Ab initio calculations for the H 2 interaction with the dimers of Si͑100͒2 ϫ1 show properties of the potential surface in qualitative agreement with the model, but its dynamics differs quantitatively from the experimental results. ͓S0163-1829͑96͒01732-8͔

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Section: Introductionmentioning

confidence: 99%

Reaction dynamics of molecular hydrogen on silicon surfaces

et al. 1996

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“…Some previous work, which has addressed a range of systems, has suggested that T-ehp coupling makes a negligible or minor contribution for the specific processes and systems investigated, 18,34,35 which included H-atoms interacting with Cu(110). 36 Other previous work, 37 some of which also focused on H-atoms interacting with metal surfaces, 38,39 suggested that ehp excitation should constitute the dominant energy loss mechanism.…”

Section: Introductionmentioning

confidence: 98%

“…Bisschler et al used a soft cube model to investigate sticking, adsorption, and absorption of H-atoms on Cu(110). 36 Hammer and co-workers 41 used a potential energy surface (PES) based on semi-empirical effective medium theory and DFT calculations to study scattering of H-atoms from Cu(111) for incidence energies (E i ) ranging up to 1.2 eV and T s up to 500 K. An important conclusion from their work was that the surface corrugation needs to be taken into account: the Baule-model fails at predicting sticking probabilities, which are affected by energy conversion from normal to parallel translational motion, and by the possibility that the H-atoms penetrate the surface even at low E i . Klamroth and Saalfrank used reduced dimensionality quantum dynamical models, mixed-quantum classical models, and the classical trajectory method to study sticking of H-atoms from Cu(100).…”

Section: Introductionmentioning

confidence: 99%

“…The use of the AIMD method circumvents the need to perform high-dimensional potential fits that capture the coupling of the H-atom translational motion with the surface phonons, as forces are calculated on the fly directly from DFT. Compared to the theoretical calculations on H-atom scattering from copper and gold surfaces 36,41,68,70 that are most relevant to the present work, the research presented here uses an improved dynamical model of the phonons, avoids inaccuracies associated with potential fits, and treats a much higher E i (5 eV) at which non-adiabatic effects should be more important. However, the computational expense of the AIMD method forces us to focus on the component of the scattering (scattering without surface penetration) that proceeds on a short time scale.…”

Section: Introductionmentioning

confidence: 99%

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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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“…The interaction of atomic hydrogen, the simplest atom, with transition metal surfaces has attracted large interest, because it is the testing ground for our understanding of surface processes. The simplicity of the adsorbate electronic structure lead to a large body of existing theoretical work on this metal-adsorbate interaction [36][37][38]. The hydrogen metal bond is relatively weak (DHðMe À HÞ < 2 eV for noble metals, and somewhat stronger DHðMe À HÞ % 2 À 3 eV for transition metals [39]).…”

Section: Introductionmentioning

confidence: 99%

Non-adiabaticity in surface chemical reactions

Hasselbrink

2009

Surface Science

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Sticking, adsorption, and absorption of atomic H on Cu(110)

Cited by 66 publications

References 28 publications

Reaction dynamics of molecular hydrogen on silicon surfaces

Reaction dynamics of molecular hydrogen on silicon surfaces

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

Non-adiabaticity in surface chemical reactions

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