Abstract
We performed a detailed experimental investigation and quantum-chemical analysis of two-photon absorption (2PA) spectra of a series of symmetrical cationic polymethines and neutral squaraines having similar structures. Degenerate 2PA spectra of these molecules are taken by using two-photon fluorescence spectroscopy and the Z-scan technique. All measurements are made with laser pulses of repetition rate in the tuning range of . Comparing 2PA spectra of polymethines and squaraines, we find that we can access considerably larger 2PA cross sections (/photon) in the squaraines owing to narrower linear absorption spectra and an increase in the density of unoccupied molecular orbitals introduced by the squaraine acceptor group in the conjugated chain.
© 2006 Optical Society of America
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