Full Quantum Calculations
of the Diffusion Rate of Adsorbates
Thiago Firmino, Roberto Marquardt, Fabien Gatti, David Zanuttini
and Wei Dong
Abstract The dynamical structure factor S(q, E) related to the scattering of particles on mobile adsorbates is evaluated quantum mechanically from the formula
proposed by van Hove (Phys. Rev. 95: 249–262, 1954) using eigenfunctions and
eigenvalues obtained with the Multiconfiguration Time Dependent Hartree method.
Three different one dimensional models for the CO/Cu(100) system and a three
dimensional model for H/Pd(111) are investigated. Results are discussed in
connection with recent
3 He spin echo experiments reported in the literature.
Keywords Quantum diffusion Á High dimensional quantum dynamics Á Heterogeneous
catalysis
1 Introduction
The motion of hydrogen atoms adsorbed on metal surfaces has been explored with
picosecond time resolution in
3 He spin-echo experiments for H/Pt(111) [1] and
H/Ru(0001) [2]. The primary quantity determined in these experiments is the
intermediate scattering function (ISF) I (q, t), where q is the wave vector related to
the momentum transferred from the scattered
3 He atoms to the hydrogen atoms
moving on the surface, and t is the time.
T. Firmino Á R. Marquardt (&)
Laboratoire de Chimie Quantique, Institut de Chimie UMR 7177 CNRS/UdS,
Université de Strasbourg, 1 rue Blaise Pascal, BP 296/R8, 67008 Strasbourg Cedex, France
e-mail: roberto.marquardt@unistra.fr
F. Gatti Á D. Zanuttini
CTMM, Institut Charles Gerhardt UMR 5253, CNRS/Université de Montpellier,
34095 Montpellier Cedex 05, France
W. Dong
Laboratoire de Chimie UMR 5182 CNRS/Ecole Normale Supérieure de Lyon,
46 Allée d’Italie, 69364 Lyon Cedex 07, France
© Springer International Publishing Switzerland 2015
M.A.C. Nascimento et al. (eds.), Frontiers in Quantum Methods and Applications
in Chemistry and Physics, Progress in Theoretical Chemistry and Physics 29,
DOI 10.1007/978-3-319-14397-2_11
177
of the Diffusion Rate of Adsorbates
Thiago Firmino, Roberto Marquardt, Fabien Gatti, David Zanuttini
and Wei Dong
Abstract The dynamical structure factor S(q, E) related to the scattering of particles on mobile adsorbates is evaluated quantum mechanically from the formula
proposed by van Hove (Phys. Rev. 95: 249–262, 1954) using eigenfunctions and
eigenvalues obtained with the Multiconfiguration Time Dependent Hartree method.
Three different one dimensional models for the CO/Cu(100) system and a three
dimensional model for H/Pd(111) are investigated. Results are discussed in
connection with recent
3 He spin echo experiments reported in the literature.
Keywords Quantum diffusion Á High dimensional quantum dynamics Á Heterogeneous
catalysis
1 Introduction
The motion of hydrogen atoms adsorbed on metal surfaces has been explored with
picosecond time resolution in
3 He spin-echo experiments for H/Pt(111) [1] and
H/Ru(0001) [2]. The primary quantity determined in these experiments is the
intermediate scattering function (ISF) I (q, t), where q is the wave vector related to
the momentum transferred from the scattered
3 He atoms to the hydrogen atoms
moving on the surface, and t is the time.
T. Firmino Á R. Marquardt (&)
Laboratoire de Chimie Quantique, Institut de Chimie UMR 7177 CNRS/UdS,
Université de Strasbourg, 1 rue Blaise Pascal, BP 296/R8, 67008 Strasbourg Cedex, France
e-mail: roberto.marquardt@unistra.fr
F. Gatti Á D. Zanuttini
CTMM, Institut Charles Gerhardt UMR 5253, CNRS/Université de Montpellier,
34095 Montpellier Cedex 05, France
W. Dong
Laboratoire de Chimie UMR 5182 CNRS/Ecole Normale Supérieure de Lyon,
46 Allée d’Italie, 69364 Lyon Cedex 07, France
© Springer International Publishing Switzerland 2015
M.A.C. Nascimento et al. (eds.), Frontiers in Quantum Methods and Applications
in Chemistry and Physics, Progress in Theoretical Chemistry and Physics 29,
DOI 10.1007/978-3-319-14397-2_11
177