Real Space Visualization of Entangled Excitonic States in Charged Molecular Assemblies
| Autor: | Pablo Merino, Jiří Doležal, Prokop Hapala, Rodrigo Cezar De Campos Ferreira, Sofia Canola, Martin Švec |
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| Přispěvatelé: | Czech Grant Agency, Charles University (Czech Republic), European Commission, Comunidad de Madrid |
| Rok vydání: | 2021 |
| Předmět: |
Condensed Matter - Mesoscale and Nanoscale Physics
Delocalization General Engineering FOS: Physical sciences General Physics and Astronomy STM-induced luminescence 02 engineering and technology 021001 nanoscience & nanotechnology 01 natural sciences PTCDA STML Entanglement Mesoscale and Nanoscale Physics (cond-mat.mes-hall) 0103 physical sciences General Materials Science Physics - Atomic and Molecular Clusters AFM Exciton Atomic and Molecular Clusters (physics.atm-clus) 010306 general physics 0210 nano-technology |
| Zdroj: | Digital.CSIC. Repositorio Institucional del CSIC instname |
| ISSN: | 1936-086X 1936-0851 |
| Popis: | 7 pags., 4 figs. Entanglement of excitons holds great promise for the future of quantum computing, which would use individual molecular dyes as building blocks of their circuitry. Studying entangled excitonic eigenstates emerging in coupled molecular assemblies in the near-field with submolecular resolution has the potential to bring insight into the photophysics of these fascinating quantum phenomena. In contrast to far-field spectroscopies, near-field spectroscopic mapping permits direct identification of the individual eigenmodes, type of exciton coupling, including excited states otherwise inaccessible in the far field (dark states). Here we combine tip-enhanced spectromicroscopy with atomic force microscopy to inspect delocalized single-exciton states of charged molecular assemblies engineered from individual perylenetetracarboxylic dianhydride (PTCDA) molecules. Hyperspectral mapping of the eigenstates and comparison with calculated many-body optical transitions reveals a second low-lying excited state of the anion monomers and its role in the exciton entanglement within the assemblies. We demonstrate control over the exciton coupling by switching the assembly charge states. Our results reveal the possibility of tailoring excitonic properties of organic dye aggregates for advanced functionalities and establish the methodology to address them individually at the nanoscale. S.C., R.C.C.F., M.Š ., and J.D. acknowledge the Czech grant agency funding no. 20-18741S and the Charles University Grant Agency project no. 910120. P.M. thanks the ERC Synergy Program (grant no. ERC-2013- SYG-610256, Nanocosmos) for financial support and the “Comunidad de Madrid” for its support to the FotoArt-CM Project (S2018/NMT-4367) through the Program of R&D activities between research groups in Technologies 2013, cofinanced by European Structural Funds. |
| Databáze: | OpenAIRE |
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