Simulating Highly Activated Sticking of H2on Al(110): Quantum versus Quasi-Classical Dynamics

• Autores: Tchakoua, Theophile; Powell, Andrew D.; Gerrits, Nick; Somers, Mark F.; Doblhoff Dier, Katharina; Busnengo, Heriberto Fabio; Kroes, Geert Jan
• Año de publicación: 2023
• Idioma: inglés
• Tipo de recurso: artículo
• Materia: SUPERFICIES; ABINITIO
• Institución: Consejo Nacional de Investigaciones Científicas y Técnicas

We evaluate the importance of quantum effects on the sticking of H2on Al(110) for conditions that are close to those of molecular beam experiments that have been done on this system. Calculations with the quasi-classical trajectory (QCT) method and with quantum dynamics (QD) are performed using a model in which only motion in the six molecular degrees of freedom is allowed. The potential energy surface used has a minimum barrier height close to the value recently obtained with the quantum Monte Carlo method. Monte Carlo averaging over the initial rovibrational states allowed the QD calculations to be done with an order of magnitude smaller computational expense. The sticking probability curve computed with QD is shifted to lower energies relative to the QCT curve by 0.21 to 0.05 kcal/mol, with the highest shift obtained for the lowest incidence energy. Quantum effects are therefore expected to play a small role in calculations that would evaluate the accuracy of electronic structure methods for determining the minimum barrier height to dissociative chemisorption for H2+ Al(110) on the basis of the standard procedure for comparing results of theory with molecular beam experiments.
Fil: Tchakoua, Theophile. Leiden University; Países Bajos
Fil: Powell, Andrew D.. Leiden University; Países Bajos
Fil: Gerrits, Nick. Leiden University; Países Bajos
Fil: Somers, Mark F.. Leiden University; Países Bajos
Fil: Doblhoff Dier, Katharina. Leiden University; Países Bajos
Fil: Busnengo, Heriberto Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Kroes, Geert Jan. Leiden University; Países Bajos