Multiconfiguration time‐dependent Hartree (MCTDH) study on rotational and diffractive inelastic molecule‐surface scattering

The multiconfiguration time‐dependent Hartree (MCTDH) method is applied 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 H₂/rectangular lattice and N₂/LiF (001) are investigated for scattering with normal incidence. The performance and reliability of the MCTDH method is critically examined with respect to the structure of the MCTDH wave function and the choice of the basis set representation. The MCTDH reproduces the fine details of the state‐to‐state transition probabilities calculated by the numerically exact close‐coupled wave packet (CCWP) method. We show that it is useful to represent two of the internal degrees of freedom by one set of single‐particle functions when these degrees are strongly coupled, or when their MCTDH‐contraction efficiency is low.