Abstract To investigate interchromophore interactions in azobenzene polymers, we have undertaken a thorough spectroscopic analysis of the azodye [(S)-3-pivaloyloxy-1-(4′-nitro- 4-azobenzene) pyrrolidine] by modeling the repeating unit of poly [(S)-3-methacryloyloxy-1- (4′-nitro-4-azobenzene) pyrrolidine) and its dimeric derivative whose synthesis is presented here. The analysis of the electronic and Raman spectra of the azodye in ...