Orientation dependence of NO sticking and scattering at Pt (100)

Müller, Helmut; Zagatta, Gunther; Böwering, N.; Heinzmann, Ulrich

doi:10.1016/0009-2614(94)00440-4

Cited by 18 publications

(14 citation statements)

References 32 publications

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“…For spectroscopic reasons, such experiments are particularly well suited to the NO molecule. [2][3][4][5][6][7][8][9][10][11][12][13] The measured features resulting from the scattering experiments cannot directly be linked to the potential energy surface. Molecular dynamics ͑MD͒ simulations can give insight how those features are connected to properties of the potential energy surface and provide detailed information on the dynamical processes of the gas-surface interaction.…”

Section: Introductionmentioning

confidence: 99%

Orientation and energy dependence of NO scattering from Pt(111)

Lahaye

Stolte

Holloway

et al. 1996

The Journal of Chemical Physics

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A classical molecular dynamics study is applied to simulate the scattering of NO from Pt͑111͒ in the energy range of 0.3-1 eV. The solid consists of a large number of crystal atoms that interact via an anharmonic nearest-neighbor potential. The NO-Pt͑111͒ interaction potential is constructed as a pairwise additive potential with a well depth of 1 eV for the N end of the molecule towards the surface and purely repulsive for the O end. The in-plane scattering results obtained with this model potential are compared with recent experiments for NO-Pt͑111͒. The angular intensity distributions, the final translational energy, as well as the rotational energy distributions with the corresponding alignment are in qualitative agreement with those experimental results. A detailed examination of the collision dynamics shows that multiple collisions with the surface results predominantly in superspecular scattering. The rotational angular momentum of the scattered molecules exhibits a preference for cartwheeling alignment and the rotational energy distributions for specular and normal exit angles can be described with a Boltzmann distribution, whereas for grazing exit angles they are distinctly non-Boltzmann. The latter structure results from a cutoff in the rotational excitation by the attraction of the well. The high rotational excitation clearly originates from molecules that initially are oriented with the O end towards the surface, whereas for the low rotational excitation this orientation preference disappears.

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Section: Introductionmentioning

confidence: 99%

Orientation and energy dependence of NO scattering from Pt(111)

Lahaye

Stolte

Holloway

et al. 1996

The Journal of Chemical Physics

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“…Thus, we target measurements at high kinetic energy to have the best chance of avoiding the obscuring effects of dynamical steering. Moreover, the experiment is further simplified at high kinetic energy as these conditions suppress sticking (20), an elementary surface process where strong orientation effects have been previously reported (21)(22)(23)(24)(25)(26)(27).…”

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confidence: 99%

Observation of orientation-dependent electron transfer in molecule–surface collisions

Bartels

Golibrzuch

Bartels

et al. 2013

Proc. Natl. Acad. Sci. U.S.A.

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Molecules typically must point in specific relative directions to participate efficiently in energy transfer and reactions. For example, Förster energy transfer favors specific relative directions of each molecule's transition dipole [Förster T (1948) Ann Phys 2(1-2):55-75] and electron transfer between gas-phase molecules often depends on the relative orientation of orbitals [Brooks PR, et al. (2007) J Am Chem Soc 129(50):15572-15580]. Surface chemical reactions can be many orders of magnitude faster than their gas-phase analogs, a fact that underscores the importance of surfaces for catalysis. One reason surface reactions can be so fast is the labile change of oxidation state that commonly takes place upon adsorption, a process involving electron transfer between a solid metal and an approaching molecule. By transferring electrons to or from the adsorbate, the process of bond weakening and/or cleavage is initiated, chemically activating the reactant [Yoon B, et al. (2005) (111) surface with the N atom oriented toward the surface. This represents a rare opportunity to investigate the steric influences on an electron transfer reaction happening at a surface.dynamics at surfaces | orientation of molecules | rotational rainbow T he measurement of the orientation dependence of reaction rates can provide a sensitive test of theories of chemical processes. Electron transfer (ET) reactions are of particular interest in this regard, both because of the fundamental issues they pose involving subtle long-range orientation-dependent interactions, and because of the importance of ET in a remarkably wide range of phenomena. Long-range ET reactions play an important role in living systems (1). They are important in catalysis on metals and zeolites (2), in rechargeable batteries, in corrosion (3), and in photosynthesis (4).On metal surfaces, an ET reaction may proceed by transient formation of a molecular anion via excitation of electronic states of the metal, often precluding a description of the reaction mechanism within an adiabatic picture based on the BornOppenheimer approximation (5, 6). As in the analogy to whaling used in naming gas-phase ET reactions, this process of an electron jump from the surface to an approaching molecule is often referred to as "harpooning" (7). There are many studies of the orientation dependence of harpooning in gas-phase reactions (8, 9), but little is known about steric influences on ET reactions during molecule-surface scattering events. An influence of N 2 O orientation on exoelectron emission has been seen for reactions at alkali surfaces (10). Mechanistic studies revealed evidence for an Eley-Rideal reaction involving an ET event (11, 12). However, theoretical considerations suggest that the ET from the solid to N 2 O is independent of N 2 O orientation (13). To our knowledge, there is no unambiguous measurement of the orientation dependence of an ET reaction at a solid surface.We have found a unique way to measure the orientation dependence of a simple ET reaction occurring when ...

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“…In the reactive NO=Pt111, the trapping probability is higher for the N end than for the O end [2]. The sticking probability of NO on reactive Ni(100) and Pt(100) also demonstrated that the N end is more reactive than the O end [3,5,7]. Moreover, clear steric effects have been observed in the gas-phase products for the (NO CO) reactions on Pt(100) [6].…”

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confidence: 96%

“…The steric effect, reactant orientation, and alignment, are of great importance in surface chemistry [1][2][3][4][5][6][7][8][9][10][11][12][13][14][15]. The stereodynamics of NO on a surface has been a particular target of several studies using various experimental approaches [1][2][3][4][5][6][7].…”

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Stereodynamics in Dissociative Adsorption of NO on Si(111)

Hashinokuchi

Okada

et al. 2008

Phys. Rev. Lett.

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We report results of our study on the surface-temperature dependence of the steric effect in the dissociative adsorption of NO on Si(111)-(7x7). Data presented here show that, at an incident energy of 58 meV, the reactive sticking probability for the N-end collision is larger than that for the O-end collision. Furthermore, this steric preference is quite sensitive to the surface temperature and the surface coverage. This study shows that the transient surface trapping into a shallow precursor well plays a key role in the stereodynamics of the dissociative adsorption at the low energy region.

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Orientation dependence of NO sticking and scattering at Pt (100)

Cited by 18 publications

References 32 publications

Orientation and energy dependence of NO scattering from Pt(111)

Orientation and energy dependence of NO scattering from Pt(111)

Observation of orientation-dependent electron transfer in molecule–surface collisions

Stereodynamics in Dissociative Adsorption of NO on Si(111)

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