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We present a comprehensive analysis of autoionization processes in Ne clusters ∼5000 atoms) after multiple valence excitations by free electron laser (FEL) radiation. Such highly excited clusters can decay non-radioactively only via energy exchange between at least two neighboring excited atoms, known as interatomic Coulombic decay (ICD). The electron emission spectra are dominated by ICD and its multistep evolution towards lower kinetic energies at the cluster surface 2p --> 3s excitation. Whereas at the bulk 2p --> 3s excitation the inelastic scattering (knock-up and knock-out) of ICD electrons is clearly observed. New decay channel is open following 2p--> 3d excitation, namely intra-Rydberg ICD, where 3d--> 3s de-excitation of an atom leads to ionization of neighboring excited atom. This intra-Rydberg ICD quenches the direct ICD and is followed by ICD cascades.
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