The Role of Molecular Arrangement on the Dispersion in Strongly Coupled Metal-Organic Hybrid Structures
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| Autores principales: | , , , , , , |
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| Formato: | Preprint |
| Publicado: |
2021
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| _version_ | 1866916377790513152 |
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| author | Rödel, Maximilian Lisinetskaya, Polina Rudloff, Maximilian Stark, Thomas Manara, Jochen Mitric, Roland Pflaum, Jens |
| author_facet | Rödel, Maximilian Lisinetskaya, Polina Rudloff, Maximilian Stark, Thomas Manara, Jochen Mitric, Roland Pflaum, Jens |
| contents | Metal-organic hybrid structures have been demonstrated a versatile platform to study primary aspects of light-matter interaction by means of emerging states comprising excitonic and plasmonic properties. Here we are studying the wave-vector dependent photo-excitations in gold layers covered by molecular films of zinc-phthalocyanine and its fluorinated derivatives (FnZnPc, with n = 0,4,8,16). These layered metal-organic samples show up to four anti-crossings in their dispersions correlating in energy with the respective degree of ZnPc fluorination. By means of complementary structural and theoretical data, we attribute the observed anti-crossings to three main scenarios of surface plasmon coupling: i) to aggregated $α$-phase regions within the FnZnPc layers at 1.75 eV and 1.85 eV , ii) to a coexisting F16ZnPc $β$-polymorph at 1.51 eV, and iii) to monomers, preferentially located at the metal interface, at 2.15 eV. Whereas energy and splitting of the monomer anti-crossings depend on strength and average tilting of the molecular dipole moments, the aggregate related anti-crossings show a distinct variation with degree of fluorination. These observations can be consistently explained by a change in FnZnPc dipole density induced by an increased lattice spacing due to the larger molecular van der Waals radii upon fluorination. The reported results prove Au/FnZnPc bilayers a model system to demonstrate the high sensitivity of exciton-plasmon coupling on the molecular alignment at microscopic length scales. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2111_09185 |
| institution | arXiv |
| publishDate | 2021 |
| record_format | arxiv |
| spellingShingle | The Role of Molecular Arrangement on the Dispersion in Strongly Coupled Metal-Organic Hybrid Structures Rödel, Maximilian Lisinetskaya, Polina Rudloff, Maximilian Stark, Thomas Manara, Jochen Mitric, Roland Pflaum, Jens Optics Metal-organic hybrid structures have been demonstrated a versatile platform to study primary aspects of light-matter interaction by means of emerging states comprising excitonic and plasmonic properties. Here we are studying the wave-vector dependent photo-excitations in gold layers covered by molecular films of zinc-phthalocyanine and its fluorinated derivatives (FnZnPc, with n = 0,4,8,16). These layered metal-organic samples show up to four anti-crossings in their dispersions correlating in energy with the respective degree of ZnPc fluorination. By means of complementary structural and theoretical data, we attribute the observed anti-crossings to three main scenarios of surface plasmon coupling: i) to aggregated $α$-phase regions within the FnZnPc layers at 1.75 eV and 1.85 eV , ii) to a coexisting F16ZnPc $β$-polymorph at 1.51 eV, and iii) to monomers, preferentially located at the metal interface, at 2.15 eV. Whereas energy and splitting of the monomer anti-crossings depend on strength and average tilting of the molecular dipole moments, the aggregate related anti-crossings show a distinct variation with degree of fluorination. These observations can be consistently explained by a change in FnZnPc dipole density induced by an increased lattice spacing due to the larger molecular van der Waals radii upon fluorination. The reported results prove Au/FnZnPc bilayers a model system to demonstrate the high sensitivity of exciton-plasmon coupling on the molecular alignment at microscopic length scales. |
| title | The Role of Molecular Arrangement on the Dispersion in Strongly Coupled Metal-Organic Hybrid Structures |
| topic | Optics |
| url | https://arxiv.org/abs/2111.09185 |