First principles studies on one-, two-, and three-photon absorption properties of a symmetric carbazole derivative both in gas phase and solution

One-, two-, and three-photon absorption spectra of a novel symmetric carbazole derivative have been calculated by applying density functional response theory, both in gas phase and in a selection of solvents with increasing polarity. The effect from surrounding solvents is described by the polarizable continuum model. The effect of the choice of geometry, as well as the exchange–correlation functional has been carefully analyzed. It is found that the Coulomb attenuation method variant of Becke’s three-parameter exchange and the Lee–Yang–Parr correlation functional (CAMB3LYP) can reproduce very well the experimental one-photon absorption lineshape. The dielectric solutions enhance both one- and multi-photon absorption properties. Possible explanations for the discrepancy between calculated and experimental three-photon absorption cross sections have been analyzed in details. The calculation suggests that the possible involvement of excite-state absorption in the experimental measurement cannot be ruled out.