MULTICONFIGURATION TIME-DEPENDENT HARTREE (MCTDH) STUDY ON ROTATIONALAND DIFFRACTIVE INELASTIC MOLECULE-SURFACE SCATTERING

The multiconfiguration time-dependent Hartree (MCTDH) method is applie d to rotational and diffractive inelastic molecule-corrugated surface scattering, The molecule is treated as a rigid rotor, hence there are five degrees of freedom included in the calculation. The model systems H-2/rectangular lattice and N-2/LiF (001) are investigated for scatte ring with normal incidence. The performance and reliability of the MCT DH method is critically examined with respect to the structure of the MCTDH wave function and the choice of the basis set representation. Th e MCTDH reproduces the fine details of the state-to-state transition p robabilities calculated by the numerically exact close-coupled wave pa cket (CCWP) method. We show that it is useful to represent two of the internal degrees of freedom by one set of single-particle functions wh en these degrees are strongly coupled, or when their MCTDH-contraction efficiency is low. (C) 1996 American Institute of Physics.