The family of centropolyindanes are created by edge-wise fusing of the cyclopentane ring of several indane units (D. Kuck, Chemical Reviews 2006, 106, 4885-4925). Centropolyindane chemistry could become a starting point to completely novel supramolecular aggregates and supermolecular carbocyclic architectures. The aim of this proposal is to simultaneously measure the INS and Raman spectra of seven centropolyindanes and to analyse the spectra with the aid of CASTEP. The unusual fused-ring motifs present in the materials may provide new group frequencies characteristic of these structures. This group of compounds will let us see: (i) how the progressive addition of indane units to the core, (ii) geometrical isomerisation and (iii) substitution of the bridgehead carbons modifies the spectra.