Anisotropic Photo-Physical Properties of Plexcitons in Strongly Coupled Metal-Organic Thin Films
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arXiv
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| Autori principali: | , , , , , , , |
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| Natura: | Preprint |
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2024
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| _version_ | 1866911065118343168 |
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| author | Rödel, Maximilian Philipp, Luca Nils Kim, Jin Hong Lehmann, Matthias Stolte, Matthias Mitric, Roland Würthner, Frank Pflaum, Jens |
| author_facet | Rödel, Maximilian Philipp, Luca Nils Kim, Jin Hong Lehmann, Matthias Stolte, Matthias Mitric, Roland Würthner, Frank Pflaum, Jens |
| contents | 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 $\vecμ$ and the surface plasmon wavevector $\vec{k}_x$ 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2409_01210 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Anisotropic Photo-Physical Properties of Plexcitons in Strongly Coupled Metal-Organic Thin Films Rödel, Maximilian Philipp, Luca Nils Kim, Jin Hong Lehmann, Matthias Stolte, Matthias Mitric, Roland Würthner, Frank Pflaum, Jens Optics Chemical Physics 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 $\vecμ$ and the surface plasmon wavevector $\vec{k}_x$ 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. |
| title | Anisotropic Photo-Physical Properties of Plexcitons in Strongly Coupled Metal-Organic Thin Films |
| topic | Optics Chemical Physics |
| url | https://arxiv.org/abs/2409.01210 |