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Anisotropic Photo-Physical Properties of Plexcitons in Strongly Coupled Metal-Organic Thin Films

2024/09/02 by Maximilian Rödel, Luca Nils Philipp, Rödel, Maximilian +13 · 2 citations
Engineering · Materials Science · Physics and Astronomy · #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Molecular Junctions and Nanostructures #Optics (physics.optics) #Organic and Molecular Conductors Research #Spectroscopy and Quantum Chemical Studies

paper · pdf · doi:10.48550/arxiv.2409.01210

openalex publication_date 2024/09/02 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28

Abstract

Exciton plasmon polaritons have gained increasing interests over recent years due to their versatile properties emerging by the underlying light-matter coupling and making them potential candidates for new photonic applications. We have advanced this concept by studying thin films of laterally aligned J-type aggregates of self-assembled tetra-bay phenoxy-dendronized perylene bisimide (PBI) molecules, arranged in a helical manner of three strains on a silver surface. As a result of the interaction between the uniformly aligned dipole moments and the surface plasmons of a thin silver layer underneath, the excitonic state at 1.94 eV evolves into dispersions in absorption and emission, both characterized by a distinct anisotropy. The coupling constant defined by the scalar product of the transition dipole moment μ and the surface plasmon wavevector kx shows a pronounced two-fold rotational symmetry with values between almost 0 to 28 meV. Complementary TD-DFT calculations of the angular dependent absorption and photoluminescence provide insights in the coherent energy exchange between the excitonic and plasmonic sub-systems. Additionally, power dependent PL studies yield first evidence that the diffusion length of the coupled exciton-plasmon polaritons exceeds that of the mere Frenkel state in neat PBI by at least one order of magnitude. Our results not only demonstrate the possibility to control the photo-physical properties of strongly coupled states by their spatially anisotropic light-matter interaction but also reveal innovative strategies to influence opto-electronic device operation by the directional transport of hybrid state energy.

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