CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, 11 BeiYiTiao, ZhongGuanCun, Beijing 100190, China.
College of Chemistry and Materials Science, Anhui Normal University, Wuhu 241002, China.
Nano Lett. 2021 Apr 28;21(8):3573-3580. doi: 10.1021/acs.nanolett.1c00596. Epub 2021 Apr 8.
The exploitation of strong light-matter interactions in chiral plasmonic nanocavities may enable exceptional physical phenomena and lead to potential applications in nanophotonics, information communication, etc. Therefore, a deep understanding of strong light-matter interactions in chiral plasmonic-excitonic (plexcitonic) systems constructed by a chiral plasmonic nanocavity and molecular excitons is urgently needed. Herein, we systematically studied the strong light-matter interactions in gold nanorod-based chiral plexcitonic systems assembled on DNA origami. Rabi splitting and anticrossing behavior were observed in circular dichroism spectra, manifesting chiroptical characteristic hybridization. The bisignate line shape of the circular dichroism (CD) signal allows the accurate discrimination of hybrid modes. A large Rabi splitting of ∼205/∼199 meV for left-handed/right-handed plexcitonic nanosystems meets the criterion of strong coupling. Our work deepens the understanding of light-matter interactions in chiral plexcitonic nanosystems and will facilitate the development of chiral quantum optics and chiroptical devices.
在手性等离子体激元纳米腔中的强光物质相互作用的开发可能会实现特殊的物理现象，并导致在纳米光子学、信息通讯等领域的潜在应用。因此，迫切需要深入了解由手性等离子体纳米腔和分子激子构建的手性等离子体激元-激子（plexcitonic）系统中的强光物质相互作用。在这里，我们系统地研究了组装在 DNA 折纸结构上的基于金纳米棒的手性 plexcitonic 系统中的强光物质相互作用。圆二色性光谱中观察到拉比分裂和反交叉行为，表现出手征光学特征杂化。圆二色性（CD）信号的双峰线形状允许对杂化模式进行准确区分。对于左手/右手 plexcitonic 纳米系统，拉比分裂约为 205/199meV，满足强耦合的标准。我们的工作加深了对手性 plexcitonic 纳米系统中光物质相互作用的理解，并将促进手征量子光学和手征光学器件的发展。
