Bending of cilia and flagella occurs when axonemal dynein molecules on one side of the axoneme produce force and move toward the microtubule (MT) minus end. These dyneins are then pulled back when ...the axoneme bends in the other direction, meaning oscillatory back and forth movement of dynein during repetitive bending of cilia/flagella. There are various factors that may regulate the dynein activity, e.g. the nexin-dynein regulatory complex, radial spokes, and central apparatus. In order to understand the basic mechanism of dynein’s oscillatory movement, we constructed a simple model system composed of MTs, outer-arm dyneins, and crosslinks between the MTs made of DNA origami. Electron microscopy (EM) showed pairs of parallel MTs crossbridged by patches of regularly arranged dynein molecules bound in two different orientations, depending on which of the MTs their tails bind to. The oppositely oriented dyneins are expected to produce opposing forces when the pair of MTs have the same polarity. Optical trapping experiments showed that the dynein-MT-DNA-origami complex actually oscillates back and forth after photolysis of caged ATP. Intriguingly, the complex, when held at one end, showed repetitive bending motions. The results show that a simple system composed of ensembles of oppositely oriented dyneins, MTs, and inter-MT crosslinkers, without any additional regulatory structures, has an intrinsic ability to cause oscillation and repetitive bending motions.
Nanoarchitectural control of matter is crucial for next-generation technologies. DNA origami templates are harnessed to accurately position single molecules; however, direct single molecule evidence ...is lacking regarding how well DNA origami can control the orientation of such molecules in three-dimensional space, as well as the factors affecting control. Here, we present two strategies for controlling the polar (θ) and in-plane azimuthal (ϕ) angular orientations of cyanine Cy5 single molecules tethered on rationally-designed DNA origami templates that are physically adsorbed (physisorbed) on glass substrates. By using dipolar imaging to evaluate Cy5′s orientation and super-resolution microscopy, the absolute spatial orientation of Cy5 is calculated relative to the DNA template. The sequence-dependent partial intercalation of Cy5 is discovered and supported theoretically using density functional theory and molecular dynamics simulations, and it is harnessed as our first strategy to achieve θ control for a full revolution with dispersion as small as ±4.5°. In our second strategy, ϕ control is achieved by mechanically stretching the Cy5 from its two tethers, being the dispersion ±10.3° for full stretching. These results can in principle be applied to any single molecule, expanding in this way the capabilities of DNA as a functional templating material for single-molecule orientation control. The experimental and modeling insights provided herein will help engineer similar self-assembling molecular systems based on polymers, such as RNA and proteins.
While DNA origami is a popular and versatile platform, its structural properties are still poorly understood. In this study we use solid-state nanopores to investigate the ionic permeability and ...mechanical properties of DNA origami nanoplates. DNA origami nanoplates of various designs are docked onto solid-state nanopores where we subsequently measure their ionic conductance. The ionic permeability is found to be high for all origami nanoplates. We observe the conductance of docked nanoplates, relative to the bare nanopore conductance, to increase as a function of pore diameter, as well as to increase upon lowering the ionic strength. The honeycomb lattice nanoplate is found to have slightly better overall performance over other plate designs. After docking, we often observe spontaneous discrete jumps in the current, a process which can be attributed to mechanical buckling. All nanoplates show a nonlinear current–voltage dependence with a lower conductance at higher applied voltages, which we attribute to a physical bending deformation of the nanoplates under the applied force. At sufficiently high voltage (force), the nanoplates are strongly deformed and can be pulled through the nanopore. These data show that DNA origami nanoplates are typically very permeable to ions and exhibit a number of unexpected mechanical properties, which are interesting in their own right, but also need to be considered in the future design of DNA origami nanostructures.
Self-assembly of anisotropic metal nanoparticles serves as an effective bottom-up route for the nanofabrication of novel artifacts. However, there still are many challenges to rationally manipulate ...anisotropic particles due to the size and geometric restrictions. To avoid the aggregation and mishybridization from DNA sticky-end-guided assembly in buffer solution, in this work, we utilized a cation-controlled surface diffusion strategy to the spatial arrangement of gold nanorods (AuNRs) into 1D and 2D arrays by using DNA origami tiles as binding frames on the solid–liquid interface through π–π stacking interactions. To facilitate the further manipulation of those patterns, a novel pattern transfer method was introduced to transfer the arrays of AuNRs from a liquid to a dry ambient environment with high yield and minor structural damage. The results demonstrated a successful strategy of DNA origami-assisted, large-scale assembly of AuNRs for constructing complex superstructures with potential applications in the nanofabrication of plasmonic and electronic devices.
During immune responses, activating ligands would trigger dynamic spatiotemporal organization of immunoreceptors at the cell interface, governing the fate and effector functions of immune cells. To ...understand the biophysical mechanisms of immunoreceptor signaling, diverse tools, including DNA technologies, have been developed to manipulate receptor–ligand interactions during the immune activation process. With great capability in the controllable assembly of biomolecules, functional DNA-based precise arrangement of immune molecules at cell interfaces has provided a powerful means in revealing the principles of immunoreceptor triggering, even at the single-molecule level. In addition, precisely regulating immunoreceptor–ligand interactions with functional DNA has been applied in immunotherapies of major diseases. This Perspective will focus on the recent advances in exploring immunoreceptor signaling with functional DNA as the molecular tool as well as the applications of functional DNA mediated regulation of immunoreceptor activation. We also outline the challenges and opportunities of applying functional DNA in immune modulation and immunotherapy.
Deployable geometries are finite auxetic structures that preserve their overall shapes during expansion and contraction. The topological behaviors emerge from intricately arranged elements and their ...connections. Despite the considerable utility of such configurations in nature and in engineering, deployable nanostructures have never been demonstrated. Here a deployable flight ring, a simplified planar structure of Hoberman sphere is shown, using DNA origami. The DNA flight ring consists of topologically assembled six triangles in two layers that can slide against each other, thereby switching between two distinct (open and closed) states. The origami topology is a trefoil knot, and its auxetic reconfiguration results in negative Poisson's ratios. This work shows the feasibility of deployable nanostructures, providing a versatile platform for topological studies and opening new opportunities for bioengineering.
This work introduces the first deployable nanoscale geometry using DNA origami. This planar structure is inspired by Hoberman sphere and the topology is a trefoil knot. The DNA flight ring can switch between open and closed states, showing auxetic reconfiguration with negative Poisson's ratios.
DNA nanotechnology allows for the realization of complex nanoarchitectures in which the spatial arrangements of different constituents and most functions can be enabled by DNA. When optically active ...components are integrated in such systems, the resulting nanoarchitectures not only provide great insights into the self-assembly of nanoscale elements in a systematic way but also impart tailored optical functionality to DNA origami. In this Letter, we demonstrate DNA-assembled multilayer nanosystems, which can carry out coordinated and reversible sliding motion powered by DNA fuels. Gold nanoparticles cross-link DNA origami filaments to define the configurations of the multilayer nanoarchitectures as well as to mediate relative sliding between the neighboring origami filaments. Meanwhile, the gold nanoparticles serve as optical probes to dynamically interact with the fluorophores tethered on the filaments, rendering in situ detection of the stepwise sliding processes possible. This work seeds the basis to implement DNA-assembled complex optical nanoarchitectures with programmability and addressability, advancing the field with new momentum.
In 2009, Jonoska, Seeman and Wu showed that every graph admits a route for a DNA reporter strand, that is, a closed walk covering every edge either once or twice, in opposite directions if twice, and ...passing through each vertex in a particular way. This corresponds to showing that every graph has an edge-outer embedding, that is, an orientable embedding with some face that is incident with every edge. In the motivating application, the objective is such a closed walk of minimum length. Here we give a short algorithmic proof of the original existence result, and also prove that finding a shortest length solution is NP-hard, even for 3-connected cubic (3-regular) planar graphs. Independent of the motivating application, this problem opens a new direction in the study of graph embeddings, and we suggest several problems emerging from it.
Chiral Systems Made from DNA Winogradoff, David; Li, Pin‐Yi; Joshi, Himanshu ...
Advanced science,
03/2021, Letnik:
8, Številka:
5
Journal Article
Recenzirano
Odprti dostop
The very chemical structure of DNA that enables biological heredity and evolution has non‐trivial implications for the self‐organization of DNA molecules into larger assemblies and provides limitless ...opportunities for building functional nanostructures. This progress report discusses the natural organization of DNA into chiral structures and recent advances in creating synthetic chiral systems using DNA as a building material. How nucleic acid chirality naturally comes into play in a diverse array of situations is considered first, at length scales ranging from an individual nucleotide to entire chromosomes. Thereafter, chiral liquid crystal phases formed by dense DNA mixtures are discussed, including the ongoing efforts to understand their origins. The report then summarizes recent efforts directed toward building chiral structures, and other structures of complex topology, using the principle of DNA self‐assembly. Discussed last are existing and proposed functional man‐made nanostructures designed to either probe or harness DNA's chirality, from plasmonics and spintronics to biosensing.
This progress report discusses the natural organization of DNA into chiral structures and recent advances in creating synthetic chiral systems using DNA as a building material. The topics covered include chirality of biological DNA systems at all scales, liquid crystal phases of dense DNA solutions, programmable chirality in self‐assembled DNA nanostructures, and DNA‐based plasmonic and spintronic systems.
Plasmonic nanoantennas allow for enhancing the spontaneous emission, altering the emission polarization, and shaping the radiation pattern of quantum emitters. A critical challenge for the ...experimental realizations is positioning a single emitter into the hotspot of a plasmonic antenna with nanoscale accuracy. We demonstrate a dynamic light–matter interaction nanosystem enabled by the DNA origami technique. A single fluorophore molecule can autonomously and unidirectionally walk into the hotspot of a plasmonic nanoantenna along a designated origami track. Successive fluorescence intensity increase and lifetime reduction are in situ monitored using single-molecule fluorescence spectroscopy, while the fluorophore walker gradually approaches and eventually enters the plasmonic hotspot. Our scheme offers a dynamic platform, which can be used to develop functional materials, investigate intriguing light–matter interaction phenomena, and serve as prototype system for examining theoretical models.
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