The results of a femtosecond laser investigation of the photophysical
and photochemical properties of the DCM styryl laser dye molecule are
reported. Femtosecond pump-probe experiments (absorption/gain spectros
copy using a white light continuum and up-conversion fluorescence spec
troscopy) show a red shift of the gain and emission spectra and a blue
shift of the S-1-->S-N absorption band only due to a fast reorganizat
ion of the solvent cage around the highly polar fluorescent first sing
let excited state of DCM. This first complete study (spontaneous emiss
ion, gain and absorption) of DCM with a pump-probe intercorrelation fu
nction around 300 fs (FWHM) demonstrates that the hypothesis of a tran
sition from a locally excited (LE) to a twisted intramolecular charge
transfer (TICT) state is not valid for DCM.