N2 dissociative adsorption on Ru(0001):: The role of energy loss

被引:50
作者
Diekhöner, L [1 ]
Mortensen, H [1 ]
Baurichter, A [1 ]
Jensen, E [1 ]
Petrunin, VV [1 ]
Luntz, AC [1 ]
机构
[1] Odense Univ, Syddansk Univ, Inst Fys, DK-5230 Odense M, Denmark
关键词
D O I
10.1063/1.1413746
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
New molecular beam experiments on the dissociation probability S-0 for N-2 on Ru(0001) are presented. These are in general agreement with prior measurements and exhibit very unusual behavior; a very slow increase of S-0 with incident kinetic energy E and the fact that S-0 is still only similar to 10(-3) at incident energies considerably above the barrier. A simple dynamical model is developed to describe this unusual sticking behavior. The key aspect is that there is considerable energy loss Delta from E upon initial impact with the surface (principally to the lattice) and only E-Delta is then available to surmount the activation barrier in the exit channel. Using experimentally measured values of Delta from scattering experiments gives good qualitative agreement of this model with the measured S-0. One implication of the strong energy loss is that there is an apparent violation of detailed balance when comparing only the reactive fluxes of activated adsorption and associative desorption. (C) 2001 American Institute of Physics.
引用
收藏
页码:9028 / 9035
页数:8
相关论文
共 39 条
  • [1] A QUANTUM-MECHANICAL MECHANISM FOR THE DISSOCIATIVE CHEMISORPTION OF N-2 ON METAL-SURFACES
    ASSCHER, M
    BECKER, OM
    HAASE, G
    KOSLOFF, R
    [J]. SURFACE SCIENCE, 1988, 206 (03) : L880 - L887
  • [2] TUNNELING MECHANISM FOR THE DISSOCIATIVE CHEMISORPTION OF N-2 ON METAL-SURFACES
    ASSCHER, M
    HAASE, G
    KOSLOFF, R
    [J]. VACUUM, 1990, 41 (1-3) : 269 - 271
  • [3] DETAILED BALANCING AND QUASI-EQUILIBRIUM IN ADSORPTION OF HYDROGEN ON COPPER
    CARDILLO, MJ
    BALOOCH, M
    STICKNEY, RE
    [J]. SURFACE SCIENCE, 1975, 50 (02) : 263 - 278
  • [4] Dissociative adsorption of N2 on Ru(0001):: A surface reaction totally dominated by steps
    Dahl, S
    Törnqvist, E
    Chorkendorff, I
    [J]. JOURNAL OF CATALYSIS, 2000, 192 (02) : 381 - 390
  • [5] The synthesis of ammonia over a ruthenium single crystal
    Dahl, S
    Taylor, PA
    Tornqvist, E
    Chorkendorff, I
    [J]. JOURNAL OF CATALYSIS, 1998, 178 (02) : 679 - 686
  • [6] Role of steps in N2 activation on Ru(0001)
    Dahl, S
    Logadottir, A
    Egeberg, RC
    Larsen, JH
    Chorkendorff, I
    Törnqvist, E
    Norskov, JK
    [J]. PHYSICAL REVIEW LETTERS, 1999, 83 (09) : 1814 - 1817
  • [7] The dissociation of diatomic molecules at surfaces
    Darling, GR
    Holloway, S
    [J]. REPORTS ON PROGRESS IN PHYSICS, 1995, 58 (12) : 1595 - 1672
  • [8] Coverage dependence of activation barriers:: Nitrogen on Ru(0001)
    Diekhöner, L
    Mortensen, H
    Baurichter, A
    Luntz, AC
    [J]. JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A-VACUUM SURFACES AND FILMS, 2000, 18 (04): : 1509 - 1513
  • [9] Dynamics of high-barrier surface reactions:: Laser-assisted associative desorption of N2 from Ru(0001)
    Diekhöner, L
    Mortensen, H
    Baurichter, A
    Luntz, AC
    Hammer, B
    [J]. PHYSICAL REVIEW LETTERS, 2000, 84 (21) : 4906 - 4909
  • [10] Observation of metastable atomic nitrogen adsorbed on Ru(0001)
    Diekhöner, L
    Baurichter, A
    Mortensen, H
    Luntz, AC
    [J]. JOURNAL OF CHEMICAL PHYSICS, 2000, 112 (05) : 2507 - 2515