Rotational alignment in associative desorption of H2 from Pd(100)

Rotational effects in dissociation of H2 on Pd(111): Quantum and classical study

“…19 In the panels on the right it is clear that the QC calculations of A 0 (2) (J) predict a nonmonotonous variation with J: it first increases, passes through a maximum, and then decreases in agreement with experimental and theoretical results for H 2 /Pd(100). 3,4,11 The origin of this behavior, which is the most pronounced for low energies, can also be traced back to the results presented in Fig. 8 for E i ϭ55 meV.…”

“…Moreover, the latter effects also produce a nonmonotonous dependence of the quadrupole alignment A 0 (2) on J, as observed in associative desorption experiments on H 2 /Pd(100). 3,4 Note that the importance of rotational hindering and of adiabatic energy transfer from rotation to translation is not restricted to the H 2 /Pd(111) system. They also play a prominent role for H 2 /Pd(100) 9,11 and for dissociation of D 2 on Cu͑111͒ ͑above threshold͒.…”

“…During the last several years, rotational effects in adsorption/desorption dynamics of H 2 on Pd surfaces have been studied experimentally [1][2][3][4][5][6] and theoretically. [7][8][9][10][11] This interest is due to the fact that rotational effects help to identify reaction mechanisms 1,6 and can be used to gauge the orientational dependence of the molecule-surface potential energy surface ͑PES͒.…”

“…[7][8][9][10][11] This interest is due to the fact that rotational effects help to identify reaction mechanisms 1,6 and can be used to gauge the orientational dependence of the molecule-surface potential energy surface ͑PES͒. 3,4,11 Experiments carried out for H 2 /Pd(111) with molecular beams of different mean rotational energies showed that at low translational energies, rotation hinders dissociative adsorption. 1 These experimental results confirmed the prediction of previous six-dimensional quantum calculations ͓for H 2 /Pd(100)] carried out by Gross and co-workers, 7 who interpreted their results in terms of the steering effect: 7,12 steering is suppressed for high values of the rotational quantum number J, because a rotating molecule is less easily oriented to a geometry favorable for reaction.…”

Towards a specific reaction parameter density functional for reactive scattering of H2 from Pd(111)

“…Also other low index surfaces have been studied intensively. Experimental data is available for Pd(100) [28][29][30][31] and Pd(110), 32 and theoretical studies have also been performed on Pd(100) [33][34][35][36][37] and Pd(110). 32,[38][39][40] This work is organized as follows: In Sec.…”