期刊
ACS NANO
卷 15, 期 2, 页码 2292-2300出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c08274
关键词
chirality; strong coupling; plexcitons; chiral J-aggregates; plasmonic nanoparticles
类别
资金
- National Key Research and Development Program of China [2016YFA0301300, 2017YFA0303400]
- Fundamental Research Funds for the Central Universities
- National Natural Science Foundation of China [11574035, 11774036, 91850104]
- Fund of State Key Laboratory of Information Photonics and Optical Communications (Beijing University of Posts and Telecommunications), P.R. China
- NSFC-RGC [11861161002]
This study experimentally investigates the optical chirality of plexcitonic systems, made up of composite metal nanoparticles and chiral J-aggregates, in the strong coupling regime. Mode splitting and anticrossing behavior are observed in both the circular dichroism (CD) and extinction spectra of the hybrid nanosystems. The research provides insights into the modification of extinction and optical chirality in hybrid systems due to the formation of plexcitons, and proposes a criterion for strong plasmon-exciton interaction based on mode splitting in CD spectra.
Understanding the unique characteristics of plexcitons, hybridized states resulting from the strong coupling between plasmons and excitons, is vital for both fundamental studies and practical applications in nano-optics. However, the research of plexcitons from the perspective of chiral optics has been rarely reported. Here, we experimentally investigate the optical chirality of plexcitonic systems consisting of composite metal nanoparticles and chiral J-aggregates in the strong coupling regime. Mode splitting and anticrossing behavior are observed in both the circular dichroism (CD) and extinction spectra of the hybrid nanosystems. A large mode splitting (at zero detuning) of up to 136 meV/214 meV in CD/extinction measurements confirms that the systems attain the strong coupling regime. This phenomenon indicates that the formation of plexcitons modifies not only the extinction but also the optical chirality of the hybrid systems. We develop a quasistatic theory to elucidate the chiral optical responses of hybrid systems. Furthermore, we propose and justify a criterion of strong plasmon-exciton interaction: the mode splitting in the CD spectra (at zero detuning) is larger than half of that in the extinction spectra. Our findings give a chiral perspective on the study of strong plasmon-exciton coupling and have potential applications in the chiral optical field.
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