Using the DNA origami technique, we constructed a DNA nanodevice functionalized with small interfering RNA (siRNA) within its inner cavity and the chemotherapeutic drug doxorubicin (DOX), intercalated in the DNA duplexes. The incorporation of disulfide bonds allows the triggered mechanical opening and release of siRNA in response to intracellular glutathione (GSH) in tumors to knockdown genes key to cancer progression. Combining RNA interference and chemotherapy, the nanodevice induced potent cytotoxicity and tumor growth inhibition, without observable systematic toxicity. Given its autonomous behavior, exceptional designability, potent antitumor activity and marked biocompatibility, this DNA nanodevice represents a promising strategy for precise drug design for cancer therapy.

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.

Metal nanoarchitectures fabrication based on DNA assembly has attracted a good deal of attention. DNA nanotechnology enables precise organization of nanoscale objects with extraordinary structural programmability. The spatial addressability of DNA nanostructures and sequence-dependent recognition allow functional elements to be precisely positioned; thus, novel functional materials that are difficult to produce using conventional methods could be fabricated. This review focuses on the recent development of the fabrication strategies toward manipulating the shape and morphology of metal nanoparticles and nanoassemblies based on the rational design of DNA structures. DNA-mediated metallization, including DNA-templated conductive nanowire fabrication and sequenceselective metal deposition, etc., is briefly introduced. The modifications of metal nanoparticles (NPs) with DNA and subsequent construction of heterogeneous metal nanoarchitectures are highlighted. Importantly, DNA-assembled dynamic metal nanostructures that are responsive to different stimuli are also discussed as they allow the design of smart and dynamic materials. Meanwhile, the prospects and challenges of these shape-and morphology-controlled strategies are summarized.

We report strong plasmon–exciton coupling in bimetallic nanorings and nanocuboids, and demonstrate nanoring possesses larger enhanced electric field distribution, which enables to couple with more excitons, resulting to a larger Rabi splitting.

Shape complementarity is of paramount importance in molecular recognition, but has rarely been adopted in the selfassembly of colloidal particles, especially in the case of nanoparticles of different shapes. Here, we demonstrated a simple, yet powerful strategy for fabricating gold nanoring-based heterogeneous nanostructures (AuNR-HNs) with well-defined geometries and high yield. The assembly of various geometries of AuNR-HNs is modulated by the shape complementarity of plasmonic nanorings and nanospheres. We also present experimental evidence of dark quadrupolar ring mode excitation in AuNR-HNs through singleparticle optical measurements. Our strategy will be beneficial in the study of nanoparticle assembly, photonic element interaction, and the development of plasmon-based optical devices.

Life has evolved numerous elegant molecular machines that recognize biological signals and affect mechanical changes precisely to achieve specific and versatile biofunctions. Inspired by nature, synthetic molecular machines could be designed rationally to realize nanomechanical operations and autonomous computing. We constructed logic-gated plasmonic nanodevices through coassembly of two gold nanorods (AuNRs) and computing elements on a tweezer-shaped DNA origami template. After recognition of various molecular inputs, such as DNA strands, glutathione, or adenosine, the geometry and plasmonic circular dichroism (CD) signals of the AuNR-origami nanodevices produced corresponding changes. Then we designed and characterized a set of modular Boolean logic-gated nanodevices (YES, NOT, AND, OR) and proceeded to construct a complicated 3-input circuit capable of performing Boolean OR-NOT-AND operations. Our plasmonic logic devices transduced external inputs into conformational changes and near-infrared (NIR) chiral outputs. This DNA-based self-assembly strategy holds great potential for applications in programmable optical modulators, molecular information processing, and bioanalysis.

Using the DNA origami technique, we constructed a DNA nanodevice functionalized with small interfering RNA (siRNA) within its inner cavity and the chemotherapeutic drug doxorubicin (DOX), intercalated in the DNA duplexes. The incorporation of disulfide bonds allows the triggered mechanical opening and release of siRNA in response to intracellular glutathione (GSH) in tumors to knockdown genes key to cancer progression. Combining RNA interference and chemotherapy, the nanodevice induced potent cytotoxicity and tumor growth inhibition, without observable systematic toxicity. Given its autonomous behavior, exceptional designability, potent antitumor activity and marked biocompatibility, this DNA nanodevice represents a promising strategy for precise drug design for cancer therapy.

No abstract