Two-Photon Absorption in a Conformationally Twisted D-π-A Oligomer : A Synergic Photosensitizing Approach for Multiphoton Lithography

Abstract : A comparative study of the linear and nonlinear optical properties of a novel triphenylamine–pyrimidine alternated oligomer and its corresponding V-shaped quadrupolar monomer is presented. Both chromophores strikingly exhibit the same spectral shape when considering their respective one- and two-photon absorption spectra. This effect was attributed to a weak interchromophore coupling within the oligomer which exhibits a highly distorted geometry resulting in a strong reduction of the effective conjugation length. The recursive implementation of nine monomers into a three-dimensional architecture leads however to a cooperative enhancement of the two-photon absorption (2PA) cross-section with a δMAX of 5093 GM at 800 nm. This very high 2PA ability has been oriented to improve the two-photon induced polymerization efficiency of a bicomponent photoinitiator system implying a hexaarylbiimidazole used as a H-abstractor and an aliphatic amine used as a H-donor. The photosensitizing mechanism is investigated and we clearly show that the intrinsic photoinitiation efficiency of the oligomer is increased by a factor 3 as compared to its corresponding monomer. We therefore demonstrate that such a two-photon sensitizing strategy leads to a synergy effect combining a higher photoinitiation reactivity and a very large two-photon absorption cross-section.
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Jean-Pierre Malval, Sylvain Achelle, Loïc Bodiou, Arnaud Spangenberg, Laura Chia Gomez, et al.. Two-Photon Absorption in a Conformationally Twisted D-π-A Oligomer : A Synergic Photosensitizing Approach for Multiphoton Lithography. Journal of Materials Chemistry C, Royal Society of Chemistry, 2014, 2 (37), pp.7869-7880. ⟨10.1039/C4TC00841C⟩. ⟨hal-01089207⟩

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