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The reflection and Kramers–Kronig absorption spectra have been obtained from the monoclinic and triclinic polymorphs of a squarylium dye, 2,4‐bis(4‐diethylamino‐2‐hydroxy phenyl) cyclobutadienediylium‐1,3‐diolate. The extremely different optical responses were found to arise from two molecular singlet transitions of essentially long axis polarization. Successful application of a four oscillator molecular exciton–polariton theory required the use of point charge densities rather than point dipoles in an extension of the theory which employed both interactions between the two singlets as well as a frequency dependent lattice damping. An intermolecular charge transfer transition is also assigned.

Influence of crystal fields on the quasimetallic reflection spectra of crystals: Optical spectra of polymorphs of a squarylium dye