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. 2019 Nov 27;10(1):5394.
doi: 10.1038/s41467-019-13444-3.

A rotary plasmonic nanoclock

Ling Xin  1 , Chao Zhou  1 , Xiaoyang Duan  1   2 , Na Liu  3   4
Affiliations

A rotary plasmonic nanoclock

Ling Xin et al. Nat Commun. .

Abstract

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.

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Conflict of interest statement

The authors declare no competing interests.

Figures

Fig. 1
Fig. 1
Stepwise plasmonic nanoclock. a Schematic of the rotary plasmonic nanoclock for stepwise rotation. The DNA origami structure consists of three connected components: a bundle, a ring track, and a plate. One gold nanorod (AuNR) is assembled on the bundle, serving as rotor. The other AuNR is assembled on the back surface of the plate, serving as stator. Sixteen footholds in eight pairs are evenly distributed around the origami ring, forming a circular track. The two feet (black) extended from the bundle can bind to any pair of the footholds. b Foothold arrangement around the ring track. fh1, fh1′–fh8, fh8′ are shown in 8 different colors. θ is defined as the angle between the rotor and stator AuNRs. Each rotation step corresponds to Δθ = π/8. c Working principle of the stepwise rotation (AuNRs are not shown) powered by DNA fuels based on a “release and capture” mechanism. It is enabled by addition of corresponding blocking strands and removal strands through toehold-mediated strand displacement reactions. d Transmission electron microscopy (TEM) image of the DNA origami structures. Inset: enlarged view of a representative DNA structure, scale bar 20 nm. e TEM image of the plasmonic nanoclocks.
Fig. 2
Fig. 2
Optical characterizations of the stepwise rotation process. a Circular dichroism (CD) spectra measured at various rotation angles θ. b CD intensities at 732 nm extracted from the spectra in Fig. 2a as a function of θ during a full-turn clockwise rotation process. c Stepwise rotations along clockwise (black) and counterclockwise (red) directions, demonstrating good reversibility. The experiments were carried out on 2 samples, source data are provided with the paper.
Fig. 3
Fig. 3
Autonomous plasmonic nanoclock. a Schematic of the rotary plasmonic nanoclock for autonomous rotation. The main DNA origami structure is taken from the stepwise plasmonic nanoclock design with modifications. The feet are two 8–17 DNAzyme strands (green) extended from the two ends of the bundle. RNA substrates (purple) are assembled around the ring track as footholds. Upper (black) and lower (black-red) locking strands are extended from the bundle and fh1, fh1′, respectively, to fix the rotor at starting position 1-1′. b Working principle of the autonomous rotation powered by DNAzyme-RNA interactions in the presence of Mg2+.
Fig. 4
Fig. 4
In situ optical characterizations of the autonomous rotation process. a Time-course CD measurement at 732 nm for clockwise autonomous rotation. For each sample, the rotor is initially fixed at position 1-1′. The times for adding removal strands r to activate the DNAzyme feet and blocking strands B1 to unlock the rotor from position 1-1′ are indicated in the plot. The arrangements of the substrates around the track are varied for different samples as illustrated in the schematic on the right (right half is shown). b Control experiment 1, in which two substrates are omitted around the ring track. Track arrangement 1-2-x–x-5 (light blue) means that there are no substrates at fh3 (fh3′) and fh4 (fh4′). c Control experiment 2, in which one substrate is omitted around the ring track. Track arrangement 1-2-3-x-5 (blue) means that there is no substrate at fh4 (fh4′). d Time-course CD measurement at 732 nm for counterclockwise autonomous rotation. The arrangements of the substrates around the track are varied for different samples as illustrated in the schematic on the right (left half is shown). The experiments were carried out on 14 samples, source data are provided with the paper.
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