Anisotropy of third-order nonlinear optical properties in di-n-butyl fluorescein derivatives was investigated by electroabsorption spectroscopy. In a series of fluoresceins, the derivatives with Cl substitution at phenyl ring presented a new intense absorption band at the wavelength range from 550 to 620 nm, which is at longer wavelength side of the main absorption band in other derivatives. This new absorption band was attributed to intramolecular charge transfer transition due to Cl substitution at the phenyl ring, according to the spectral profile of electroabsorption which was proportional to the second derivative of linear absorption spectrum. Polarization dependence of normalized absorption coefficient was about 2:1 at the main absorption band in all derivatives. However, in the charge transfer transition band, the polarization dependence was about 1:1,2, suggesting that the charge transfer direction is nearly perpendicular to the otpical transition. This result is consistent with structural aspect that the charge transfer direction is located along to the bond between the Cl-substituted phenyl ring and condensed ring, while the optical transition is along to the longitudinal axis of the condensed ring.
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