Fullerene and azafullerene films were studied by electron energy loss spectroscopy in reflection geometry. Compared to C60, (C59N)2 multilayers show additional vibrational modes that are characteristic of the dimer structure. The (C59N)2 is semiconductor-like and giant optically allowed excitonic transitions are found in the gap in drastic contrast with C60. The azafullerene monolayer on Cu(111) no longer shows the presence of dimers, indicating monomer adsorption. Similarly to C60, azafullerene molecules in contact with the metal substrate receive a transferred charge between two and three electrons. However, the C59N appears more covalently bound to Cu because it decomposes when heated above 660 K while C60 only desorbs.
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