Dissociative adsorption of H2 on Cu(100) : Fixed-site calculations for impact at hollow and top sites

The reaction of H2 on Cu(100) is studied using a wave-packet method to solve a four-dimensional quantum mechanical model for impact on the high-symmetry hollow and top sites. The potential energy surface (PES) is a fit to the results of density functional calculations treating a periodic overlayer of H2 on a Cu slab. The dynamics calculations include motion in the azimuthal coordinate although the PES does not depend on φ for impact on the top and hollow sites. Large dissociation probabilities (∼0.9) are found for impact at the hollow site but those for impact at the top site are lower (∼0.3). Dissociation probabilities for molecules incident with “helicoptering” motion (mj=j) are larger than those for molecules with “cartwheeling” motion (mj=0). This differs from the results of previous calculations for impact at the azimuthally corrugated bridge site which predicted comparable probabilities for the two orientations of incident molecules. The dissociation probabilities from fixed-site calculations at the...

[1]  E. Baerends,et al.  Six-dimensional quantum dynamics of dissociative chemisorption of H2 on Cu(100) , 1997 .

[2]  J. Light,et al.  Six dimensional quantum dynamics study for dissociative adsorption of H2 on Cu(111) surface , 1997 .

[3]  Alec M. Wodtke,et al.  The Stereodynamics of a Gas-Surface Reaction , 1997 .

[4]  E. Baerends,et al.  Six-dimensional quantum dynamics of dissociative chemisorption of (v=0, j=0) H2 on Cu(100). , 1997 .

[5]  E. Baerends,et al.  Dissociative adsorption of H2 on Cu(100): A four-dimensional study of the effect of rotational motion on the reaction dynamics , 1997 .

[6]  H. Kasai,et al.  Role of Rotational Motion in the Dissociative Adsorption and Associative Desorption Dynamics of D{sub 2}/Cu(111) , 1997 .

[7]  C. Rettner,et al.  Alignment of D2(v, J) desorbed from Cu(111): Low sensitivity of activated dissociative chemisorption to approach geometry , 1996 .

[8]  D. Neuhauser,et al.  DISSOCIATIVE CHEMISORPTION OF H2 ON CU(100) : A FOUR-DIMENSIONAL STUDY OF THE EFFECT OF PARALLEL TRANSLATIONAL MOTION ON THE REACTION DYNAMICS , 1996 .

[9]  H. Zacharias,et al.  Rotational corrugation in associative desorption of D2 from Cu(111) , 1996 .

[10]  B. Hammer,et al.  A comparison of quantum and classical dynamics of H2 dissociation on Cu(111) , 1996 .

[11]  E. J. Baerends,et al.  An analytical six-dimensional potential energy surface for dissociation of molecular hydrogen on Cu(100) , 1996 .

[12]  Kroes,et al.  Competition between vibrational excitation and dissociation in collisions of H2 with Cu(100). , 1996, Physical review. B, Condensed matter.

[13]  E. Baerends,et al.  Erratum: Dissociation of H2 on Cu(100): Dynamics on a new two‐dimensional potential energy surface [J. Chem. Phys. 102, 3873 (1995)] , 1995 .

[14]  G. Kroes,et al.  Application of an efficient asymptotic analysis method to molecule–surface scattering , 1995 .

[15]  M. Gostein,et al.  Survival probability of H2(v=1,J=1) scattered from Cu(110). , 1995, Physical review letters.

[16]  J. H. Zhang,et al.  Quantum adsorption dynamics of a diatomic molecule on surface: Four‐dimensional fixed‐site model for H2 on Cu(111) , 1995 .

[17]  A. Gross.  THE ROLE OF LATERAL SURFACE CORRUGATION FOR THE QUANTUM DYNAMICS OF DISSOCIATIVE ADSORPTION AND ASSOCIATIVE DESORPTION , 1995 .

[18]  C. Rettner,et al.  Quantum‐state‐specific dynamics of the dissociative adsorption and associative desorption of H2 at a Cu(111) surface , 1995 .

[19]  Scheffler,et al.  High-dimensional quantum dynamics of adsorption and desorption of H2 at Cu(111). , 1994, Physical review letters.

[20]  J. H. Zhang,et al.  Steric effect in dissociative chemisorption of hydrogen on Cu , 1994 .

[21]  S. Holloway,et al.  Rotational motion and the dissociation of H2 on Cu(111) , 1994 .

[22]  J. H. Zhang,et al.  Symmetry and rotational orientation effects in dissociative adsorption of diatomic molecules on metals: H2 and HD on Cu(111) , 1994 .

[23]  S. Holloway,et al.  Dissociation thresholds and the vibrational excitation process in the scattering of H2 , 1994 .

[24]  S. Holloway,et al.  The role of parallel momentum in the dissociative adsorption of H2 at highly corrugated surfaces , 1994 .

[25]  R. C. Mowrey.  Dissociative adsorption of H2 using the close‐coupling wave packet method , 1993 .

[26]  J. H. Zhang,et al.  Quantum dynamics studies of adsorption and desorption of hydrogen at a Cu(111) surface , 1993 .

[27]  W. Miller,et al.  Time‐independent quantum dynamics for diatom–surface scattering , 1993 .

[28]  C. Rettner,et al.  Effect of rotation on the translational and vibrational energy dependence of the dissociative adsorption of D2 on Cu(111) , 1993 .

[29]  C. Rettner,et al.  Interaction dynamics of hydrogen at a Cu(111) surface , 1993 .

[30]  C. Rettner,et al.  From quantum-state-specific dynamics to reaction rates: the dominant role of translational energy in promoting the dissociation of D2 on Cu(111) under equilibrium conditions , 1993 .

[31]  J. H. Zhang,et al.  An algebraic variational approach to dissociative adsorption of a diatomic molecule on a smooth metal surface , 1992 .

[32]  S. Holloway,et al.  Angular and vibrational effects in the sticking and scattering of H2 , 1992 .

[33]  R. Dixon,et al.  Grid methods for solving the Schrödinger equation and time dependent quantum dynamics of molecular photofragmentation and reactive scattering processes , 1992 .

[34]  S. Holloway,et al.  Translation-to-vibrational excitation in the dissociative adsorption of D2 , 1992 .

[35]  Auerbach,et al.  Observation of direct vibrational excitation in collisions of H2 and D2 with a Cu(111) surface. , 1992, Physical review letters.

[36]  S. Holloway,et al.  Enhanced diffraction of vibrationally excited molecules from surfaces , 1992 .

[37]  A. Hodgson,et al.  Energy transfer and vibrational effects in the dissociation and scattering of D2 from Cu (111) , 1992, Nature.

[38]  W. Miller,et al.  Calculation of the cumulative reaction probability via a discrete variable representation with absorbing boundary conditions , 1992 .

[39]  J. H. Zhang,et al.  Dissociative chemisorption of H2 on Ni surface: Time‐dependent quantum dynamics calculation and comparison with experiment , 1992 .

[40]  Auerbach,et al.  Role of vibrational and translational energy in the activated dissociative adsorption of D2 on Cu(111). , 1992, Physical review letters.

[41]  S. Holloway.  Vibrational and rotational effects in the dissociative adsorption of H2 , 1991 .

[42]  A. Hodgson,et al.  Scattering of vibrationally excited H2 from Cu(111) , 1991 .

[43]  D. Auerbach,et al.  A critical examination of data on the dissociative adsorption and associative desorption of hydrogen at copper surfaces , 1991 .

[44]  R. C. Mowrey.  Reactive scattering using efficient time‐dependent quantum mechanical wave packet methods on an L‐shaped grid , 1991 .

[45]  R. Dixon,et al.  Time-dependent quantum dynamics of reactive scattering and the calculation of product quantum state distributions — A study of the collinear F+H2(v=0) → HF(v′)+H reaction , 1991 .

[46]  B. Jackson,et al.  MIXED QUANTUM-CLASSICAL STUDIES OF H2 DISSOCIATION ON METALS : DEPENDENCE UPON MOLECULAR GEOMETRY AND DIMENSIONALITY , 1991 .

[47]  B. Hayden,et al.  Vibrational and translational energy partition and the barrier to dissociative H2 and D2 adsorption on Cu(110) , 1991 .

[48]  A. Winkler,et al.  A SEARCH FOR VIBRATIONAL CONTRIBUTIONS TO THE ACTIVATED ADSORPTION OF H2 ON COPPER , 1990 .

[49]  S. Holloway,et al.  The influence of potential energy surface topologies on the dissociation of H2 , 1990 .

[50]  S. Holloway,et al.  The dissociative adsorption of hydrogen: Two-, three-, and four-dimensional quantum simulations , 1990 .

[51]  R. Dixon,et al.  Time-dependent quantum dynamics of molecular photofragmentation processes , 1990 .

[52]  S. Holloway,et al.  A theoretical study of the dissociation of H2/Cu , 1989 .

[53]  Hayden,et al.  Coupled translational-vibrational activation in dissociative hydrogen adsorption on Cu(110). , 1989, Physical review letters.

[54]  S. Holloway,et al.  The scattering of H2 and D2 from Cu(100): vibrationally assisted dissociative adsorption , 1989 .

[55]  S. Holloway,et al.  Quantum‐mechanical scattering of H2 from metal surfaces: Diffraction and dissociative adsorption , 1988 .

[56]  D. Kouri,et al.  Close coupling‐wave packet formalism for gas phase nonreactive atom–diatom collisions , 1987 .

[57]  D. Kouri,et al.  Close‐coupling wave packet approach to numerically exact molecule–surface scattering calculations , 1986 .

[58]  D. Kouri,et al.  On a hybrid close-coupling—wave packet approach to molecular scattering , 1985 .

[59]  H. Tal-Ezer,et al.  An accurate and efficient scheme for propagating the time dependent Schrödinger equation , 1984 .

[60]  R. Kosloff,et al.  A fourier method solution for the time dependent Schrödinger equation as a tool in molecular dynamics , 1983 .

[61]  M. Feit,et al.  Solution of the Schrödinger equation by a spectral method , 1982 .

[62]  R. David,et al.  The purely “fast” distribution of H2 and D2 molecules desorbing from Cu(100) and Cu(111) surfaces , 1982 .

[63]  M. Balooch,et al.  Molecular beam study of the apparent activation barrier associated with adsorption and desorption of hydrogen on copper , 1974 .