Strong Light–Matter Interactions in Chiral Plasmonic–Excitonic Systems Assembled on DNA Origami

Abstract

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 nanorodbased 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.

Liquid crystal-templated chiral nanomaterials: from chiral plasmonics to circularly polarized luminescence

“…1b). Interestingly, nanoscale chirality can also be realized from directed self-assembly of achiral functional nanoparticles using various chiral soft templates such as DNA [22][23][24][25] , peptide and protein 26,27 , liquid crystal (LC) 1,2,28,29 , chiral polymer [30][31][32] , and organogelators [33][34][35][36][37] (Fig. 1c).…”

DNA-mediated dynamic plasmonic nanostructures: assembly, actuation, optical properties, and biological applications

“…24,30,137,166 By exploiting the programmability and scalability of DNA selfassembly, colloidal nanoparticles have been assembled into various LH or RH plasmonic structures. 30,[167][168][169][170][171] Organizing anisotropic nanoparticles such as AuNRs into asymmetric nanoassemblies, enhanced chirality can be generated compared to isotropic NP nanostructures due to the high dissymmetry factor and strong plasmon antenna effect. 169,172 As an example of utilizing AuNR dimers as dynamic plasmonic structures with chiroplasmonic activities, Liu's group demonstrated an active plasmonic nanoassembly, in which the AuNRs can perform directional, progressive and reverse nanoscale rows on 2D or 3D DNA origami after adding corresponding blocking and removal strands (Fig.…”

Recent developments in the chiroptical properties of chiral plasmonic gold nanostructures: bioanalytical applications

“…The splitting increases with an increase in the extent of coupling between excitonic molecule and chiral plasmonic nanostructures. The plasmon-like branch and exciton-like branch show transformations until the CD resonances of the two branches become synchronized, thus exhibiting anticrossing property [45].…”