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Superexciplex of Coumarin Molecules using Tunable Ti-Sapphire Laser

Certain highly polar dye molecules exhibit an additional optical gain band under pulsed laser excitation, while there is no such band under steady-state continuous wave (CW) lamp excitation. This new band is not due to an excimer, an exciplex or a two-photon fluorescence band but stems from the formation of a new molecular complex in which two excited molecules remain associated with a solvent molecule acting as a bridge. In this paper, the characteristics of superexciplexes of four related coumarin molecules are presented. All molecules were excited using a tunable Ti-sapphire laser pulse 10 ns in width. The distinct difference between the amplified spontaneous emission (ASE) spectra obtained with tunable laser and tunable lamp excitation demonstrated that twisted intramolecular charge transfer (TICT) conformations might also assist in the formation of these superexciplexes.