A great challenge for nanotechnology is to controllably organize anisotropic nanomaterials into well-defined three-dimensional superstructures with customized properties. Here we successfully constructed anisotropic Au nanorod (AuNR) helical superstructures (helices) with tailored chirality in a programmable manner. By designing the 'X' pattern of the arrangement of DNA capturing strands (15nt) on both sides of a two-dimensional DNA origami template, AuNRs functionalized with the complementary DNA sequences were positioned on the origami and were assembled into AuNR helices with the origami intercalated between neighboring AuNRs. Left-handed (LH) and right-handed (RH) AuNR helices were conveniently accomplished by solely tuning the mirrored-symmetric 'X' patterns of capturing strands on the origami. The inter-rod distance was precisely defined as 14 nm and inter-rod angle as 45°, thus a full helix contains 9 AuNRs with its length up to about 220 nm. By changing the AuNR/origami molar ratio in the assembly system, the average number of AuNR in the helices was tuned from 2 to 4 and 9. Intense chiroptical activities arose from the longest AuNR helices with a maximum anisotropy factor of ∼0.02, which is highly comparable to the reported macroscopic AuNR assemblies. We expect that our strategy of origami templated assembly of anisotropic chiral superstructures would inspire the bottom-up fabrication of optically active nanostructures and shed light on a variety of applications, such as chiral fluids, chiral signal amplification, and fluorescence combined chiral spectroscopy.

Discrete three-dimensional (3D) plasmonic nanoarchitectures with well-defined spatial configuration and geometry have aroused increasing interest, as new optical properties may originate from plasmon resonance coupling within the nanoarchitectures. Although spherical building blocks have been successfully employed in constructing 3D plasmonic nanoarchitectures because their isotropic nature facilitates unoriented localization, it still remains challenging to assemble anisotropic building blocks into discrete and rationally tailored 3D plasmonic nanoarchitectures. Here we report the first example of discrete 3D anisotropic gold nanorod (AuNR) dimer nanoarchitectures formed using bifacial DNA origami as a template, in which the 3D spatial configuration is precisely tuned by rationally shifting the location of AuNRs on the origami template. A distinct plasmonic chiral response was experimentally observed from the discrete 3D AuNR dimer nanoarchitectures and appeared in a spatial-configuration-dependent manner. This study represents great progress in the fabrication of 3D plasmonic nanoarchitectures with tailored optical chirality.

Hydrogels are generally thought to be formed by nano-to micrometre-scale fibres or polymer chains, either physically branched or entangled with each other to trap water. Although there are also anisotropic hydrogels with apparently ordered structures, they are essentially polymer fibre/discrete polymer chains-based network without exception. Here we present a type of polymer-free anisotropic lamellar hydrogels composed of 100-nm-thick water layers sandwiched by two bilayer membranes of a self-assembled nonionic surfactant, hexadecylglyceryl maleate. The hydrogels appear iridescent as a result of Bragg's reflection of visible light from the periodic lamellar plane. The particular lamellar hydrogel with extremely wide water spacing was used as a soft two-dimensional template to synthesize singlecrystalline nanosheets in the confined two-dimensional space. As a consequence, flexible, ultrathin and large area single-crystalline gold membranes with atomically flat surface were produced in the hydrogel. The optical and electrical properties were detected on a single gold membrane.