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• W4385240446 abstract "Coherent energy exchange between plasmons and excitons has attracted considerable interest from researchers worldwide because of their potential applications in enhanced optical processes, quantum information processing and quantum devices, artificial light harvesting, digital data storage, chemical and biological sensing, and so forth. The energy exchange between a plasmon and an exciton shows a strong dependence on various plasmonic and excitonic parameters. Here, we investigate the role of a subtle change in the chemical structure of an exciton-forming dye in controlling plasmon–exciton interaction at the nanoscale. The only difference between the two exciton-forming dyes used in this study is that one of them (Cy78) has an ethyl group on its polymethine chain, but the other (Cy75) does not. The two plexciton hybrids of the J-aggregates of Cy78 and Cy75 with the same gold nanorod are expected to show very similar plasmon–exciton interactions. However, using ensemble-level extinction as well as single-particle-level scattering spectroscopy, we reveal that, contrary to our expectations, two plexciton systems show drastically different plasmon–exciton coupling strengths. Further investigations into the origin of this unexpected observation using fluorescence spectroscopy and atomic force microscopy, complemented by density functional calculations, reveal that Cy75 exclusively exists in trans-conformation, while the presence of the ethyl substituent in Cy78 gives rise to the coexistence of cis- and trans-conformations. The presence of cis-isomers leads to the enhancement of the overall dipole moment of Cy78 J-aggregates and thereby enhancing the Rabi splitting of its plexciton hybrid by ∼100% compared to Cy75-plexciton. This comprehensive study clearly demonstrates how even an apparently “innocent” and extremely subtle change in the structure of an exciton-forming dye can drive nanoscale plasmon–exciton coupling from one coupling regime to another." @default.
• W4385240446 created "2023-07-26" @default.
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• W4385240446 date "2023-07-24" @default.
• W4385240446 modified "2023-09-25" @default.
• W4385240446 title "Subtle Structural Change in the Exciton-Forming Dye Drives Plasmon–Exciton Interaction Involving Gold Nanorods into the Strong Coupling Regime: Implications for Enhanced Optical Processes" @default.
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• W4385240446 doi "https://doi.org/10.1021/acsanm.3c01537" @default.
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