Tuning the two- photon absorption response of quadrupolar organic molecules

Egbert Zojer, D. Beljonne, T. Kogej, H. Vogel, S. R. Marder, J. W. Perry, J. L. Brédas

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We apply correlated quantum-chemical techniques to study the origin of the large two-photon absorption (TPA) cross sections, δ, in stilbene derivatives in which electron-donating and electron-withdrawing substituents provide a quadrupolar charge-transfer arrangement. An additional field created by a set of point charges is used to systematically modify the ground-state polarization to determine its consequences for the TPA response. The effect on the molecular structure can be quantified by the evolution of the π-bond-order alternation (π-BOA) of the conjugated backbone. For moderate ground-state polarizations, a marked increase of the TPA response occurs; for large polarizations, δ peaks and then drops dramatically. Insight into the origin of this evolution is gained by comparing the values of δ obtained via the converged sum-over-states approach to the results of a simple three-state model
Original languageEnglish
Article number3646
Number of pages14
JournalThe Journal of Chemical Physics
Issue number9
Publication statusPublished - 2002


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