The efficiency of the multiconfigurational time-dependent Hartree (MCTDH) method for calculating the initial-state selected dissociation probability of H-2(v=0,j=0) on Cu(100) is investigated. The MCTDH method is shown to be significantly more efficient than standard wave packet methods. A large number of single-particle functions is required to converge the initial-state selected reaction probability for dissociative adsorption. Employing multidimensional coordinates in the MCTDH ansatz (mode combination) is found to be crucial for the efficiency of these MCTDH calculations. Perspectives towards the application of the MCTDH approach to study dissociative adsorption of polyatomic molecules on surfaces are discussed. (C) 2004 American Institute of Physics.