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MO: Fachverband Molekülphysik

MO 27: Ultrafast Dynamics III and High-harmonic Generation (joint session MO/A)

MO 27.7: Vortrag

Freitag, 15. März 2024, 16:00–16:15, HS 3044

Observation of HHG from organic molecular crystals — •Falk-Erik Wiechmann1, Samuel Schöpa1, Alexander Villinger2, Dieter Bauer1, and Franziska Fennel11Institute of Physics, Rostock, Germany — 2Institute of Chemistry, Rostock, Germany

This project aims at a detailed understanding of the harmonic generation process in large organic molecules in the crystalline phase. Unlike previous studies, which were limited to small molecules in the gas phase, we introduce organic molecular crystals as a novel target for HH spectroscopy, taking advantage of the inherent molecular alignment. Unlike in gas phase experiments, neighboring molecules in organic crystals experience a weak but finite coupling, leading to 'solid like' features, e.g. a delocalization of the electronic states over several unit cells. With a fundamental 4000 nm mid-IR beam reaching 6 TW/cm2 we demonstrate that HHG up to the order of 17 is possible without imposing physical damage. When the fundamental driving polarization is rotated, maxima of harmonic emission occur at polarization directions parallel to connecting axes between neighboring molecules, reflecting the crystal structure. Despite the linearly polarized driving field, the emitted harmonics exhibit elliptical polarization with a main axis different from the fundamental polarization direction.

Keywords: High harmonic generation; Organic molecular crystals; Pentacene; Molecular alignment; Elliptical polarization

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