Abstract

Femtosecond pump–probe experiments performed on squaraines demonstrate strong couplings between the first excited state and high-lying two-photon states. The experimental data agree well with our earlier quantum many-electron calculations based on multiple-excited configuration interactions. We show that high-lying two-photon states in squaraines are critically important to understanding the observed third-order optical properties and that two-level models are inadequate even for molecules with negative third-order optical susceptibilities.

© 1994 Optical Society of America

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