The third-order optical polarizabilities (gamma) of a new homologous series of oligomeric squaraines of the indole series (monomer-pentamer) and of corresponding monomers were investigated by degenerate four wave mixing (DFWM) at 1064 nm and related to results from two-photon absorption experiments in an energy range from 1.75 to 3.2 eV. Important two-photon contributions can be deduced to vibronic coupling and the influence to (gamma) has been considered within a four-level model. The nature of the subchromophore interaction within the oligomers can succesfully be described as mainly electrostatic within the framework of simple exciton coupling theory.
Walter Grahn, Ulf Lawrentz, Katarzyna Lukaszuk, Ruediger Wortmann, Andreas Feldner, Dieter Scherer, Markus Schwoerer, Juergen Bendig, Siegrun Helm, Ina Dix, Peter Jones
We have designed and synthesized donor/acceptor substituted hexatriences 10,11, in which the configuration is locked by a hexahydroanthracene frame. Donors and acceptors of varying strength were introduced. In order to assess the potential of our merocyanines 10,11 for NLO and photorefractive (PR) applications, we have measured their linear and nonlinear optical properties and determined the NLO and PR figures-of- merit (FOMs), respectively. The merocyanine 10d exhibits a very large Kerr FOM. The thermal stability of the new merocyanines 10,11 is sufficiently high for photonic applications. In order to investigate and to correlate the bond length alternation of our oligonenes 10,11 with linear and nonlinear optical properties we have carried out x-ray structure determinations.
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