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We analyze the vibrational properties of diamondoid compounds via Ramanspectroscopy. The compounds are interconnected with carbon-carbon single bondsthat exhibit exceptionally large bond lengths up to 1.71 A. Attractivedispersion interactions caused by well-aligned intramolecular H--H contactsurfaces determine the overall structures of the diamondoid derivatives. Thestrong van-der-Waals interactions alter the vibrational properties of thecompounds in comparison to pristine diamondoids. Supported bydispersion-corrected density functional theory (DFT) computations, we analyzeand explain their experimental Raman spectra with respect to unfunctionalizeddiamondoids. We find a new set of dispersion-induced vibrational modescomprising characteristic CH/CH$_{2}$ vibrations with exceptionally highenergies. Further, we find structure-induced dimer modes that are indicative ofthe size of the dimers.

Vibrational signatures of diamondoid dimers with large intramolecular London dispersion interactions