Low-lying relaxation satellites give rise to ultrafast electron dynamics following outer-valence ionization of a molecular system. To demonstrate the impact of such satellites, the evolution of the electronic cloud after sudden removal of an electron from the highest occupied molecular orbital (HOMO) of the organic unsaturated nitroso compound 2-nitroso[1,3]oxazolo[5,4-d][1,3]oxazole is traced in real time and space using ab initio methods only. Our results show that the initially created hole charge remains stationary but on top of it the system reacts by an ultrafast pi-pi(*) excitation followed by a cyclic excitation-de-excitation process which leads to a redistribution of the charge. The pi-pi(*) excitation following the removal of the HOMO electron takes place on a subfemtosecond time scale and the period of the excitation-de-excitation alternations is about 1.4 fs. In real space the processes of excitation and de-excitation represent ultrafast delocalization and localization of the charge. The results are analyzed by simple two- and three-state models.