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A combined experimental and theoretical study of the two‐photon absorption (2PA) properties of a series of quadrupolar molecules possessing a highly electron‐rich heterocyclic core, pyrrolo[3,2‐b]pyrrole, is presented. In agreement with quantum‐chemical calculations, large 2PA cross‐section values, σ2PA≈102–103 GM (1 GM=1050 cm4 s photon−1), are observed at wavelengths of 650–700 nm, which correspond...
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