Laser induced thermal desorption of hydrogen from Zr(0001): Relationship to water dissociation and hydrogen dissolution

摘要

On metals such as Zr, during hydrogen exposure, dissolution competes with desorption; this competition can be probed by thermal desorption at different heating rates. In the case of desorption from preadsorbed hydrogen, only ～1% of the hydrogen can be desorbed even at heating rates of > 10~(10)Ks~(-1). Recent measurements of the dynamics of hydrogen released by water dissociation on Zr(0001) [G. Bussiere, M. Musa, P.R. Norton, K. Griffiths, A.G. Brolo, J.W. Hepburn, J. Chem. Phys. 124 (2006) 124704] have shown that the desorbing hydrogen originates from the recombinative desorption of adsorbed H-atoms and that over 25% of the water collisions lead to hydrogen desorption. To gain further insight into the desorption and dissolution of hydrogen and in an attempt to resolve the paradox of the different desorption yields from H_2 vs. H_2O exposures, we report new measurements of the laser induced thermal desorption (LITD) of hydrogen from Zr(0001) at initial temperatures down to 90 K. The low temperature was chosen because work function measurements suggested that hydrogen adsorbed into only the outermost (surface site) of the two available adsorption sites (surface and subsurface), from which we postulated much more efficient desorption at high heating rates compared to desorption from the sub-surface sites. However, hydrogen desorption by LITD from Zr(0001) at 90 K still only accounts for 1% of the adsorbed species, the remainder dissolving into the bulk at LITD heating rates. The different yields alluded to above remain unexplained (Bussiere, 2006).