Influence of the flux of H2 and D2 molecules on kinetics of low-temperature (down to 5 K) adsorption on the W(110) surface

被引:12
作者
Chuikov, BA [1 ]
Osovskii, VD [1 ]
Ptushinskii, YG [1 ]
Sukretnyi, VG [1 ]
机构
[1] Natl Acad Sci Ukraine, Inst Phys, UA-03650 Kiev 39, Ukraine
关键词
adsorption kinetics; deuterium; hydrogen molecule; low index single crystal surfaces; physical adsorption; sticking; tungsten;
D O I
10.1016/S0039-6028(00)00962-6
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
The molecular beam method is applied to study the kinetics of H-2 and D-2 adsorption on the W(1 1 0) surface with the substrate temperature T-S similar to 5 K as a function of the molecular flux F. The character of the effect of flux changes on the adsorption kinetics is essentially different in the cases of H-2 and D-2 adsorption. In the H-2 case, the increase of F from 5 x 10(12) to 2 x 10(14) molecules/cm(2)s modifies the coverage dependence of the sticking probability S(theta) both qualitatively and quantitatively, i.e., (i) the initial sticking probability S-0 increases more than by a factor of two; (ii) the saturation coverage theta (S) considerably increases; (iii) the monotonic (for the lowest F) dependence S(theta) transforms into a dependence with a maximum whose height grows as F increases. In the case of D-2 adsorption, the changes of F in approximately the same range produce relatively weak effect on the adsorption kinetics. In particular, both S-0 and theta (S) are changed insignificantly. The increase of S-0 with rising F is assumed to be caused by the interaction of H-2 molecules in the intrinsic precursor state which leads to the nucleation of the 2D condensed phase. The greater F the higher the nucleation probability. The 2D condensation suppresses the themodesorption from the precursor state and thus leads to the increase of S-0. The growth of theta (S) with increasing F is associated with the instability, for T-S similar to 5 K, of the physisorbed H-2 layer whose dynamically equilibrium coverage increases as F rises. The appearance of a maximum in the S(theta) dependence can be explained by greater efficiency of the energy exchange between the incident H-2 molecules and the surface under the formation of a weakly bound molecular adlayer. The revealed distinctions in the character of the molecular flux influence on the kinetics of H-2 and D-2 adsorption for T-S similar to 5 K are associated with differing quantum properties of these molecules, namely, by the deeper position of the zero-point vibrational level for the heavier D-2 molecule. (C) 2001 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:143 / 150
页数:8
相关论文
共 29 条
[1]   ADSORPTION AND DESORPTION-KINETICS WITH NO PRECURSOR TRAPPING - HYDROGEN AND DEUTERIUM ON W(100) [J].
ALNOT, P ;
CASSUTO, A ;
KING, DA .
SURFACE SCIENCE, 1989, 215 (1-2) :29-46
[2]   TRAPPING OF MOLECULAR-HYDROGEN AT SURFACES VIA TRANSLATIONAL-ROTATIONAL ENERGY-CONVERSION [J].
ANDERSSON, S ;
HARRIS, J .
PHYSICAL REVIEW B, 1983, 27 (01) :9-14
[3]   ADSORPTION OF HYDROGEN ON TUNGSTEN - A PRECURSOR PATH PLUS DIRECT ADSORPTION [J].
BERGER, HF ;
RESCH, C ;
GROSSLINGER, E ;
EILMSTEINER, G ;
WINKLER, A ;
RENDULIC, KD .
SURFACE SCIENCE, 1992, 275 (1-2) :L627-L630
[4]   Adsorption dynamics for para- and n-hydrogen on Pt(110): Rotational state resolved sticking coefficients [J].
Beutl, M ;
Riedler, M ;
Rendulic, KD .
CHEMICAL PHYSICS LETTERS, 1996, 256 (1-2) :33-36
[5]   Adsorption dynamics for CO, CO-clusters and H2 (D2) on rhodium(111) [J].
Beutl, M ;
Lesnik, J ;
Rendulic, KD .
SURFACE SCIENCE, 1999, 429 (1-3) :71-83
[6]   Strong rotational effects in the adsorption dynamics of H-2/Pd(111): Evidence for dynamical steering [J].
Beutl, M ;
Riedler, M ;
Rendulic, KD .
CHEMICAL PHYSICS LETTERS, 1995, 247 (03) :249-252
[7]  
BOSOV VS, 1973, UKR FIZ ZH, V18, P1568
[8]  
CHRISTOPOULOS C, 1988, INF MENTAL HLTH J, V9, P272, DOI 10.1002/1097-0355(198824)9:4<272::AID-IMHJ2280090403>3.0.CO
[9]  
2-M
[10]   LOW-TEMPERATURE STUDIES OF ADSORPTION OF GASES ON METALS [J].
CHUIKOV, BA ;
OSOVSKII, VD ;
PTUSHINSKII, YG ;
SUKRETNYI, VG .
SURFACE SCIENCE, 1989, 213 (2-3) :359-370