Beljonne, D.

Br\ue9das, J.-L.

Marder, S.R.

Perry, J.W.

Pond, S.J.K.

Shuai, Z.

Vogel, H.

Wenseleers, Wim

Zojer, E.

Abstract: A comparative study of the two\u2010photon absorption (TPA) properties of octupolar compounds and their dipolar one\u2010dimensional counterparts is presented on the basis of correlated quantum\u2010chemical calculations. The roles of dimensionality and symmetry are first discussed on the basis of a simple exciton picture where the ground\u2010state and excited\u2010state wavefunctions of three\u2010arm octupolar systems are built from a linear combination of the corresponding single\u2010arm wavefunctions. This model predicts a factor of 3 increase in the TPA cross section in the limiting case of three independent charge\u2010transfer pathways. When taking into account the full chemical structures of representative octupolar molecules, the results of the calculations indicate that a much larger enhancement associated with an increase in dimensionality and delocalization can be achieved when the core of the chromophore allows significant electronic coupling among the individual arms. These theoretical predictions are in agreement with the experimental determination of the TPA cross sections for crystal violet and the related compound, brilliant green, and suggest new strategies for the design of conjugated materials with large TPA cross sections

Institutional Repository Universiteit Antwerpen

Role of dimensionality on the two-photon absorption response of conjugated molecules: the case of octupolar compounds

Role of dimensionality on the two-photon absorption response of conjugated molecules: the case of octupolar compounds

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Institutional Repository Universiteit Antwerpen