Atom–surface diffraction: a trajectory description

Guantes, Raúl; Sanz, Ángel S.; Margalef-Roig, J.; Miret‐Artés, Salvador

doi:10.1016/j.surfrep.2004.02.001

Cited by 98 publications

(116 citation statements)

References 316 publications

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“…During the last two decades its usefulness has been demonstrated in the determination of numerous surface structures. [6][7][8][9][10][11] The quantitative interpretation of Hediffraction is, however, limited as the He-surface interaction potential is not known accurately. An accurate calculation of the He-surface interaction requires a quantitative description of both short range repulsive forces dominated by electronic exchange and Coulomb interactions and of the long range van der Waals interaction due to electronic correlation.…”

Section: Introductionmentioning

confidence: 99%

Diffraction of helium on MgO(100) surface calculated from first-principles

Martínez-Casado

Usvyat

Mallia

et al. 2014

Phys. Chem. Chem. Phys.

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Section: Introductionmentioning

confidence: 99%

Diffraction of helium on MgO(100) surface calculated from first-principles

Martínez-Casado

Usvyat

Mallia

et al. 2014

Phys. Chem. Chem. Phys.

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“…It provides us with an insight at a local level of the stream, but does not say anything about how a particular point-like particle evolves when it starts from a certain initial position in the corresponding configuration space. Within this approach, quantum trajectories (QTs) or streamlines are mainly obtained through any of two approaches [3]: synthetic [3][4][5] and analytic [6,7]. Within the former, QTs are computed after solving simultaneously the quantum Hamilton-Jacobi equation and the continuity one, while in the latter (used in this work) one starts from Schrödinger's equation and then the QTs are obtained from the phase of the wave function.…”

Section: Introductionmentioning

confidence: 99%

Investigating transition state resonances in the time domain by means of Bohmian mechanics: The F+HD reaction

Sanz¹,

López‐Durán²,

González‐Lezana³

2012

Chemical Physics

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In this work, we investigate the existence of transition state resonances on atom-diatom reactive collisions from a timedependent perspective, stressing the role of quantum trajectories as a tool to analyze this phenomenon. As it is shown, when one focusses on the quantum probability current density, new dynamical information about the reactive process can be extracted. In order to detect the effects of the different rotational populations and their dynamics/coherences, we have considered a reduced two-dimensional dynamics obtained from the evolution of a full three-dimensional quantum time-dependent wave packet associated with a particular angle. This reduction procedure provides us with information about the entanglement between the radial degrees of freedom (r, R) and the angular one (γ), which can be considered as describing an environment. The combined approach here proposed has been applied to study the F+HD reaction, for which the FH+D product channel exhibits a resonance-mediated dynamics.

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“…One particular example is physisorption and scattering of helium atoms on oxide surfaces. In the last two decades the latter process, employing molecular-beam techniques, has been developed into a powerful tool for the analysis of surface structure and dynamics [4][5][6][7][8]. It is particularly useful for studying insulating surfaces, such as MgO [4,9].…”

mentioning

confidence: 99%

Approaching an exact treatment of electronic correlations at solid surfaces: The binding energy of the lowest bound state of helium adsorbed on MgO(100)

et al. 2014

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In this work we employ ab initio electronic structure theory at a very high level to resolve a long standing experimental controversy; the interaction between helium and the MgO (100) surface has been studied extensively by other groups, employing diverse experimental approaches. Nevertheless, the binding energy of the lowest bound state is still unclear: the existence of a state at around −5.5 meV is well established but a state at −10 meV has also been reported. The MgO (100)-He system captures the fundamental physics involved in many adsorption problems; the weak binding is governed by long-range electronic correlation for which a fully predictive theory applicable to the solid state has been elusive. The above-mentioned experimental controversy can now be resolved on the basis of the calculations presented in this work. We performed three-dimensional vibrational dynamics calculations on a highly accurate potential-energy surface. The latter was constructed using a method which systematically approaches the exact limit in its treatment of electronic correlation. The outcome is clear: our calculations do not support the existence of a bound state around −10 meV. The interaction between molecules and crystalline surfaces is of great fundamental and technological interest and is extensively studied both experimentally and theoretically [1][2][3]. One particular example is physisorption and scattering of helium atoms on oxide surfaces. In the last two decades the latter process, employing molecular-beam techniques, has been developed into a powerful tool for the analysis of surface structure and dynamics [4][5][6][7][8]. It is particularly useful for studying insulating surfaces, such as MgO [4,9]. At close proximity the helium-surface interaction potential is dominated by the exponentially growing corrugated repulsive wall, which is a consequence of the mutual exchange repulsion between the helium and surface electron densities. The repulsive potential is two-dimensional (2D) corrugated and leads to a complicated diffraction pattern for helium scattered from the surface. In the range of intermediate He-surface distances, there exists a very shallow attractive potential due to the weak van der Waals interactions, which drops off with distance from the surface as 1/z 3 [10]. Such a potential can support several bound states (in fact several 2D bands of bound states), which correspond to vibrational levels of helium atoms physisorbed on the surface.The delicacy of the balance between different components of the helium-surface interaction makes quantitatively accurate theoretical predictions of the behavior of helium atoms on the surface extremely difficult. Standard density functional theory (DFT), which is the common tool in solid-state simulations (i.e., local-density approximation, generalized gradient approximation, or hybrids), does not capture van der Waals dispersion. In principle it can be used for calculating * r.martinezcasado@imperial.ac.uk † denis.usvyat@chemie.uni-regensburg.de the repulsive wall at th...

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Atom–surface diffraction: a trajectory description

Cited by 98 publications

References 316 publications

Diffraction of helium on MgO(100) surface calculated from first-principles

Diffraction of helium on MgO(100) surface calculated from first-principles

Investigating transition state resonances in the time domain by means of Bohmian mechanics: The F+HD reaction

Approaching an exact treatment of electronic correlations at solid surfaces: The binding energy of the lowest bound state of helium adsorbed on MgO(100)

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