The effect of surface temperature for the scattering of D2 (v = 0, j = 0)- Cu(111) system : A spherical polar TDDVR approach

Department of Physical Chemistry, Indian Association for the Cultivation of Science, Jadavpur,

Kolkata-700 032, India

E-mail : pcsa@iacs.res.in Fax : 91-33-24732805

Manuscript received 04 February 2015, accepted 06 February 2015

We have formulated a spherical polar Time Dependent Discrete Variable Representation (TDDVR) and perform four-dimensional (4D\(\otimes\)2D) as well as six-dimensional (6D) quantum dynamics on a parametrically time and temperature dependent effective Hamiltonian for D₂ (\(\upsilon\) = 0, j = 0)-Cu(111) system. Such effective potential has been derived through a mean-field approach by considering weak correlation between molecular degrees of freedom (DOFs) and surface modes, where the initial state distribution of the surface modes were introduced through Bose-Einstein Probability (BEP) factor. We demonstrate the convergence of the theoretically calculated sticking probabilities employing 4D\(\otimes\)2D quantum dynamics with increasing number of metal atoms as well as layers for rigid surface (RS) and surface at a particular temperature. It appears that the temperature dependent dissociation probabilities are exclusively dictated by those surface modes directed along Z-axis. The sticking probabilities obtained from 6D quantum dynamics are depicted as a function of initial kinetic energy (KE) of the diatom for RS and surface at 1000 K. Theoretically calculated sticking probabilities show the similar trend with the experimentally measured one