The nonlinear transmission and the excited-state absorption spectra of three fluorene derivatives exhibiting large two-photon absorptivity were measured by the third harmonic of a picosecond Nd:YAG laser. We analyzed their capability for exhibiting stimulated emission in polar solvents and found that asymmetrical fluorene compounds with a diphenylamino substituent exhibited large Stokes shifts (∼8000 cm-1), high quantum yields (∼0.9 – 1.0), and no optical gain over their entire fluorescence spectral region. In contrast, a symmetrical fluorene derivative with vinylphenylbenzothiazole substituents in positions 2 and 7 underwent lasing under one-photon excitation by use of picosecond pulsed irradiation.
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