A deep understanding of the optical properties of the chiral plexcitonic systems not only adds a new dimension to the exploration of the strong plasmon−exciton interaction but also provides a new method to design chiroptical devices. We develop a plexcitonic Born−Kuhn model to explore the strong coupling dynamics of the chiral hybrid nanostructures made of cornerstacked nanorod dimers and molecules from the chiroptical perspective. As a consequence of strong interaction between plasmons and excitons, double normal mode splittings/Rabi splittings and an anti-crossing phenomenon appear in circular dichroism (CD) spectroscopy. The character of dual plexciton (symmetric and anti-symmetric plexciton) and associated chiroptical properties have been demonstrated. The interplay between mirror symmetry breaking and plasmon−plasmon/plasmon−exciton interaction leads to an optimal configuration with the maximal chiroptical response. Moreover, chirality (of incident light) selective excitation of plexcitonic modes has been achieved by structural design. Finally, we verify our theory experimentally by synthesizing chiral plasmonic nanodimers and coating these structures with Jaggregate dye molecules.
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