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Excitonically Coupled Oligomers and Dendrimers for Two-Photon Absorption

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Photoresponsive Polymers II

Part of the book series: Advances in Polymer Science ((POLYMER,volume 214))

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.

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Authors and Affiliations

  1. Université de Lyon, Laboratoire de Chimie, CNRS – Ecole Normale Supérieure deLyon, 46 allée d'Italie, 69364, Lyon Cedex 07, France

    Chantal Andraud, Rémy Fortrie, Cyril Barsu & Henry Chermette

  2. Laboratoire de Spectrométrie Physique, CNRS UMR 5588, Université Joseph Fourier de Grenoble, Bât. E, 140 Avenue de la Physique, BP 87, 38402, St-Martin d'Hères Cedex, France

    Olivier Stéphan & Patrice L. Baldeck

  3. Chimie Physique Théorique, CNRS UMR 5180, Université Lyon, Bât. Paul Dirac (210), 43 Boulevard du 11 Novembre 1918, 69622, Villeurbanne Cedex, France

    Henry Chermette

Authors
  1. Chantal Andraud
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  2. Rémy Fortrie
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  3. Cyril Barsu
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  4. Olivier Stéphan
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  5. Henry Chermette
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  6. Patrice L. Baldeck
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Corresponding authors

Correspondence to Chantal Andraud or Patrice L. Baldeck .

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Seth R. Marder Kwang-Sup Lee

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Andraud, C., Fortrie, R., Barsu, C., Stéphan, O., Chermette, H., Baldeck, P.L. (2008). Excitonically Coupled Oligomers and Dendrimers for Two-Photon Absorption. In: Marder, S.R., Lee, KS. (eds) Photoresponsive Polymers II. Advances in Polymer Science, vol 214. Springer, Berlin, Heidelberg. https://doi.org/10.1007/12_2008_158

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