Photoresponsive Polymers II pp 149-203

Part of the Advances in Polymer Science book series (POLYMER, volume 214) | Cite as

Excitonically Coupled Oligomers and Dendrimers for Two-Photon Absorption

Chapter

Abstract

The first part of this review presents the state of the art on two-photon absorbing molecules. Earlyworks concerned the optimization of dipolar push–pull molecules. Recently, the synthesis of linearand branched centrosymmetrical quadrupolar molecules led to higher nonlinearities, but still far from reachingthe fundamental limits of molecular two-photon cross-sections.

The second part of this review summarizes our theoretical and experimental results on fluorene-basedoligomers, and branched oligomers (V-shape molecules and dendrimers). They are model molecules to investigatean alternative approach based on spatial assemblies of nonsubstituted π-electronsystems that are coupled by dipole–dipole interactions. In all geometries, two-photon absorptioncross-sections have superlinear dependencies that depend on coupling energies and oligomer sizes. Theseresults are well rationalized by an excitonic model based on N interactingthree-level systems. Analytical expressions for one-photon and two-photon energies and absorption strengthsare derived for linear oligomers. An accurate calculation of large exitonic systems is obtained by diagonalizingthe Hamiltonian operator on a reduced basis set.

Branched molecules Dendrimer Excitonic coupling Fluorene Oligomer Two-photon absorption  

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Copyright information

© Springer-Verlag Berlin Heidelberg 2008

Authors and Affiliations

  • Chantal Andraud
    • 1
  • Rémy Fortrie
    • 1
  • Cyril Barsu
    • 1
  • Olivier Stéphan
    • 2
  • Henry Chermette
    • 1
    • 3
  • Patrice L. Baldeck
    • 2
  1. 1.Université de Lyon, Laboratoire de Chimie, CNRS – Ecole Normale Supérieure deLyonLyon Cedex 07France
  2. 2.Laboratoire de Spectrométrie Physique, CNRS UMR 5588Université Joseph Fourier de Grenoble, Bât. ESt-Martin d'Hères CedexFrance
  3. 3.Chimie Physique Théorique, CNRS UMR 5180Université Lyon, Bât. Paul Dirac (210)Villeurbanne CedexFrance

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