In nano-optics, a formidable challenge remains in precise transport of a single optical nano-object along a programmed and routed path toward a predefined destination. Molecular motors in living cells that can walk directionally along microtubules have been the inspiration for realizing artificial molecular walkers. Here we demonstrate an active plasmonic system, in which a plasmonic nanorod can execute directional, progressive and reverse nanoscale walking on two or three-dimensional DNA origami. Such a walker comprises an anisotropic gold nanorod as its ‘body' and discrete DNA strands as its ‘feet'. Specifically, our walker carries optical information and can in situ optically report its own walking directions and consecutive steps at nanometer accuracy, through dynamic coupling to a plasmonic stator immobilized along its walking track. Our concept will enable a variety of smart nanophotonic platforms for studying dynamic light–matter interaction, which requires controlled motion at the nanoscale well below the optical diffraction limit.

The development of DNA nanotechnology, especially the advent of DNA origami, has made DNA ideally suited to construct nanostructures with unprecedented complexity and arbitrariness. As a fully addressable platform, DNA origami can be used to organize discrete entities in space through DNA hybridization with nanometer accuracy. Among a variety of functionalized particles, metal nanoparticles such as gold nanoparticles (AuNPs) feature an important pathway to endow DNA-origami-assembled nanostructures with tailored optical functionalities. When metal particles are placed in close proximity, their particle plasmons, i.e., collective oscillations of conduction electrons, can be coupled together, giving rise to a wealth of interesting optical phenomena. Nevertheless, characterization methods that can read out the optical responses from plasmonic nanostructures composed of small metal particles, and especially can optically distinguish in situ their minute conformation changes, are very few. Circular dichroism (CD) spectroscopy has proven to be a successful means to overcome these challenges because of its high sensitivity in discrimination of three-dimensional conformation changes. In this Account, we discuss a variety of static and dynamic chiral plasmonic nanostructures enabled by DNA nanotechnology. In the category of static plasmonic systems, we first show chiral plasmonic nanostructures based on spherical AuNPs, including plasmonic helices, toroids, and tetramers. To enhance the CD responses, anisotropic gold nanorods with larger extinction coefficients are utilized to create chiral plasmonic crosses and helical superstructures. Next, we highlight the inevitable evolution from static to dynamic plasmonic systems along with the fast development of this interdisciplinary field. Several dynamic plasmonic systems are reviewed according to their working mechanisms. We first elucidate a reconfigurable plasmonic cross structure that can execute DNA-regulated conformational changes on the nanoscale. Hosted by a reconfigurable DNA origami template, the plasmonic cross can be switched between a chiral locked state and an achiral relaxed state through toehold-mediated strand displacement reactions. This reconfigurable nanostructure can also be modified in response to light stimuli, leading to a noninvasive, waste-free, and all-optically controlled system. Taking one step further, we show that selective manipulations of individual structural species coexisting in one ensemble can be achieved using pH tuning of reconfigurable plasmonic nanostructures in a programmable manner. Finally, we describe an alternative to achieving dynamic plasmonic systems by driving AuNPs directly on origami. Such plasmonic walkers, inspired by the biological molecular motors in living cells, can generate dynamic CD responses when carrying out directional, progressive, and reverse nanoscale walking on DNA origami. We envision that the combination of DNA nanotechnology and plasmonics will open an avenue toward a new generation of functional plasmonic...

A strategy for the regulation of enzyme cascade reaction efficiency by a DNA machine in vitro is presented. Two cascade enzymes (GOx and HRP) are attached to the DNA machine, and the enzyme cascade reaction shows much higher efficiency when the two enzymes are brought closer by the DNA machine than when they are distant.

Deterministic placement and dynamic manipulation of individual plasmonic nanoparticles with nanoscale precision feature an important step toward active nanoplasmonic devices with prescribed levels of performance and functionalities at optical frequencies. In this Letter, we demonstrate a plasmonic walker couple system, in which two gold nanorod walkers can independently or simultaneously perform stepwise walking powered by DNA hybridization along the same DNA origami track. We utilize optical spectroscopy to resolve such dynamic walking with nanoscale steps well below the optical diffraction limit. We also show that the number of walkers and the optical response of the system can be correlated. Our studies exemplify the power of plasmonics, when integrated with DNA nanotechnology for realization of advanced artificial nanomachinery with tailored optical functionalities.

Ni(3+) doped NiTi layered double hydroxide (NiTi-LDH) monolayer nanosheets with a particle size of ∼ 20 nm and a thickness of ∼ 0.9 nm have been successfully prepared through a facile bottom-up approach. These NiTi-LDH monolayer nanosheets exhibit excellent supercapacitor performance, including a high specific pseudocapacitance (2310 F g(-1) at 1.5 A g(-1)) and long durability compared with bulk LDH, owing to highly exposed conductive Ni(3+) species (NiOOH) which lead to the increased mobility rate of surface charge and electrolyte-transfer. Therefore, this work is expected to take a significant step towards exploring novel 2D monolayer electrode materials with unique physical and chemical properties for applications in energy storage and conversion.

We report a DNA machine that can reversibly regulate target binding affinity on the basis of distance-dependent bivalent binding. It is a tweezer-like DNA machine that can tune the spatial distance between two ligands to construct or destroy the bivalent binding. The DNA machine can strongly bind to the target protein when the ligands are placed at an appropriate distance but releases the target when the bivalent binding is disrupted by enlargement of the distance between the ligands. This "capture-release" cycle could be repeatedly driven by single-stranded DNA without changing the ligands and target protein.

The DNA origami technique has empowered a new paradigm in plasmonics for manipulating light and matter at the nanoscale. This interdisciplinary field has witnessed vigorous growth, outlining a viable route to construct advanced plasmonic architectures with tailored optical properties. However, so far plasmonic systems templated by DNA origami have been restricted to respond to only single stimuli. Despite broad interest and scientific importance, thermal and aptamer-target regulations have not yet been widely utilized to reconfigure three-dimensional plasmonic architectures. In this Letter, we demonstrate a chiral plasmonic nanosystem integrated with split aptamers, which can respond to both thermal and aptamer-target regulations. We show that our dualresponsive system can be noninvasively tuned in a wide range of temperatures, readily correlating thermal control with optical signal changes. Meanwhile, our system can detect specific targets including adenosine triphosphate and cocaine molecules, which further enhance the optical response modulations and in turn influence the thermal tunability.

One of the fundamental challenges in nanophotonics is to gain full control over nanoscale optical elements. The precise spatiotemporal arrangement determines their interactions and collective behavior. To this end, DNA nanotechnology is employed as an unprecedented tool to create nanophotonic devices with excellent spatial addressability and temporal programmability. However, most of the current DNA-assembled nanophotonic devices can only reconfigure among random or very few defined states. Here, we demonstrate a DNA-assembled rotary plasmonic nanoclock. In this system, a rotor gold nanorod can carry out directional and reversible 360° rotation with respect to a stator gold nanorod, transitioning among 16 well-defined configurations powered by DNA fuels. The full-turn rotation process is monitored by optical spectroscopy in real time. We further demonstrate autonomous rotation of the plasmonic nanoclock powered by DNAzyme-RNA interactions. Such assembly approaches pave a viable route towards advanced nanophotonic systems entirely from the bottom-up.