An approximate quantum dynamical simulation of a large polyatomic system employing a non-empirical potential, which is calculated ``on the fly'' using an approximate Kohn--Sham approach within the local density approximation is presented. A mean-field calculation based on the Classical Separable Potential method for 41 coupled vibrational modes allows for a detailed analysis of the fast dynamics following electron photodetachment in the buckminsterfullerene anion and provides a vibrationally resolved photoelectron spectrum in a very good agreement with experiment.