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Li, Weiwei; Saleh, Ahmad; Sharma, Manas; Hünecke, Christian; Sierka, Marek; Neuhaus, Marcel; Hedewig, Lina; Bergues, Boris; Alharbi, Meshaal; ALQahtani, Hadi; Azzeer, Abdallah M.; Gräfe, Stefanie; Kling, Matthias F.; Alharbi, Abdullah F. und Wang, Zilong ORCID logoORCID: https://orcid.org/0000-0002-3975-4550 (2023): Resonance Effect in Brunel Harmonic Generation in Thin Film Organic Semiconductors. In: Advanced Optical Materials, Bd. 11, Nr. 16 [PDF, 1MB]

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Abstract

Nonlinear optical properties of organic semiconductors (OSCs) have been extensively investigated in the perturbative regime, while strong light induced high-order processes in solid-state OSCs are less studied. Here, below-threshold harmonic generation is examined, both experimentally and theoretically, in two solid-state thin film OSCs, that is, tetraphenylporphyrin and zinc tetraphenylporphyrin. Results show that the π–π* excitations of the porphyrin ring system generate the harmonic emission. The contribution of the Brunel harmonic to the 5th harmonic emission is uncovered, where the resonant 5-photon transition (S0 → S2 transition) is found to lead to an early onset of non-perturbative behavior. A similar resonance effect is expected in Brunel harmonic generation in other organic materials.

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