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Single Particle Tracking and Super-Resolution Imaging of Membrane-Assisted Stop-and-Go Diffusion and Lattice Assembly of DNA Origami
摘要： DNA nanostructures offer the possibility to mimic functional biological membrane components due to their nanometer-precise shape configurability and versatile biochemical functionality. Here we show that the diffusional behavior of DNA nanostructures and their assembly into higher order membrane-bound lattices can be controlled in a stop-and-go manner and that the process can be monitored with super-resolution imaging. The DNA structures are transiently immobilized on glass-supported lipid bilayers by changing the mono- and divalent cation concentrations of the surrounding buffer. Using DNA-PAINT super-resolution microscopy, we confirm the fixation of DNA origami structures with different shapes. On mica-supported lipid bilayers, in contrast, we observe residual movement. By increasing the concentration of NaCl and depleting MgCl2, a large fraction of DNA structures restarts to diffuse freely on both substrates. After addition of a set of oligonucleotides that enables three Y-shaped monomers to assemble into a three-legged shape (triskelion), the triskelia can be stopped and super-resolved. Exchanging buffer and adding another set of oligonucleotides triggers the triskelia to diffuse and assemble into hexagonal 2D lattices. This stop-and-go imaging technique provides a way to control and observe the diffusional behavior of DNA nanostructures on lipid membranes that could also lead to control of membrane-associated cargos.
关键词： single-particle tracking,DNA origami,diffusion,super-resolution microscopy,lipid membrane,DNA nanotechnology
更新于2025-09-23 15:23:52
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A Hybrid Carrier System Based on Origami Nanostrucutures and Layer-by-Layer Microparticles
摘要： Recent progress in DNA nanotechnology allows the fabrication of 3D structures that can be loaded with a large variety of molecular cargos and even be responsive to external stimuli. This makes the use of DNA nanostructures a promising approach for applications in nanomedicine and drug delivery. However, their low stability in the extra- and intracellular environment as well as low cellular uptake rates and release rates from endosomes into the cytoplasm hamper the efficient and targeted use of DNA nanostructures in medical applications. Here, such major obstacles are overcome by integrating DNA origami nanostructures into superordinated layer-by-layer based microparticles made from biopolymers. The modular assembly of the polymer layer allows a high-density incorporation of the DNA structures at different depth. This enables controllable protection of the DNA nanostructures over extended durations in a broad range of extra- and intracellular conditions without compromising the cell viability. Furthermore, by producing protein-complexed DNA nanostructures it is demonstrated that molecular cargo can be conveniently integrated into the developed hybrid system. This work provides the basis for a new multistage carrier system allowing for an efficient and protected transport of active agents inside responsive DNA nanostructures.
关键词： DNA origami nanostructures,drug delivery,LbL technique,hybrid carriers
更新于2025-09-23 15:23:52
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DNA origami deposition on native and passivated molybdenum disulfide substrates
摘要： Maintaining the structural fidelity of DNA origami structures on substrates is a prerequisite for the successful fabrication of hybrid DNA origami/semiconductor-based biomedical sensor devices. Molybdenum disulfide (MoS2) is an ideal substrate for such future sensors due to its exceptional electrical, mechanical and structural properties. In this work, we performed the first investigations into the interaction of DNA origami with the MoS2 surface. In contrast to the structure-preserving interaction of DNA origami with mica, another atomically flat surface, it was observed that DNA origami structures rapidly lose their structural integrity upon interaction with MoS2. In a further series of studies, pyrene and 1-pyrenemethylamine, were evaluated as surface modifications which might mitigate this effect. While both species were found to form adsorption layers on MoS2 via physisorption, 1-pyrenemethylamine serves as a better protective agent and preserves the structures for significantly longer times. These findings will be beneficial for the fabrication of future DNA origami/MoS2 hybrid electronic structures.
关键词： atomic force microscopy (AFM),molybdenum disulfide (MoS2),1-pyrenemethylamine,pyrene,DNA origami,surface modification
更新于2025-09-23 15:22:29
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Reconfigurable Plasmonic Chirality: Fundamentals and Applications
摘要： Molecular chirality is a geometric property that is of great importance in chemistry, biology, and medicine. Recently, plasmonic nanostructures that exhibit distinct chiroptical responses have attracted tremendous interest, given their ability to emulate the properties of chiral molecules with tailored and pronounced optical characteristics. However, the optical chirality of such human-made structures is in general static and cannot be manipulated postfabrication. Herein, different concepts to reconfigure the chiroptical responses of plasmonic nano- and micro-objects are outlined. Depending on the utilized strategies and stimuli, the chiroptical signature, the 3D structural conformation, or both can be reconfigured. Optical devices based on plasmonic nanostructures with reconfigurable chirality possess great potential in practical applications, ranging from polarization conversion elements to enantioselective analysis, chiral sensing, and catalysis.
关键词： plasmonics,optical spectroscopy,chirality,DNA origami,circular dichroism
更新于2025-09-23 15:19:57
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Robustness of Optical Response for Selfa??Assembled Plasmonic Metamaterials with Morphological Disorder and Surface Roughness
摘要： Bottom-up fabrication of metallized biotemplated nanostructures to form specific plasmonic nanoresonators holds promise as a means of achieving large-scale optical metamaterials. However, in contrast to top-down methods, the stochastic growth of self-assembled nanoresonators is prone to significant disorder and surface roughness, which naturally raise an important question about the robustness of their resonant properties in terms of structural imperfections. An aggregated-random-sphere model is developed to mimic the nucleated growth of metallized DNA origami assembly, leading to meta-atoms with realistic, experimentally observed morphological disorder and surface roughness. Using the well-known split-ring-resonator (SRR) motif as an example, the resonant properties of meta-atoms under different levels of roughness are investigated and a strong tolerance of optical response against morphological disorder is revealed. It is found that in SRRs, even with dramatic roughness introduced, the expected resonances are still observed, despite broadening line shapes compared to ideal smooth structure. Only for extreme disorder, which causes drastic segmentation of SRRs, does the resonant response disappear. The demonstrations are very encouraging for the prospects of bottom-up fabrication toward versatile functional metamaterials and metadevices.
关键词： self-assembly,DNA origami,metamaterials,metasurfaces,surface roughness,morphological disorder
更新于2025-09-23 15:19:57
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Dynamic actuation of DNA-assembled plasmonic nanostructures in microfluidic cell-sized compartments
摘要： Molecular motor proteins form the basis of cellular dynamics. Recently, notable efforts have led to the creation of their DNA-based mimics, which can carry out complex nanoscale motion. However, such functional analogues have not yet been integrated or operated inside synthetic cells towards the goal of realizing artificial biological systems entirely from the bottom-up. In this Letter, we encapsulate and actuate DNA-assembled dynamic nanostructures inside cell-sized microfluidic compartments. These encapsulated DNA nanostructures not only exhibit structural reconfigurability owing to their pH-sensitive molecular switches upon external stimuli, but also possess optical feedback enabled by the integrated plasmonic probes. In particular, we demonstrate the power of microfluidic compartmentalization for achieving on-chip plasmonic enantiomer separation and substrate filtration. Our work exemplifies that the two unique tools, droplet-based microfluidics and DNA technology, offering high precision on the microscale and nanoscale, respectively, can be brought together to greatly enrich the complexity and diversity of functional synthetic systems.
关键词： plasmonic enantiomer selection,droplet-based microfluidics,DNA origami,plasmonic nanostructures,pH switch
更新于2025-09-23 15:19:57
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Reconfigurable Plasmonic Nanostructures Controlled by DNA Origami
摘要： Precise surface functionalization and reconfigurable capability of nanomaterials are essential to construct complex nanostructures with specific functions. Here we show the assembly of a reconfigurable plasmonic nanostructure, which executes both conformational and plasmonic changes in response to DNA strands. In this work, different sized gold nanoparticles(AuNPs) were arranged site-specifically on the surface of a DNA origami clamp nanostructure. The opening and closing of the DNA origami clamp could be precisely controlled by a series of strand displacement reactions. Therefore, the patterns of these AuNPs could be switched between two different configurations. The observed plasmon band shift indicates the change of the plasmonic interactions among the assembled AuNPs. Our study achieves the construction of reconfigurable nanomaterials with tunable plasmon ic interactions, and will enrich the toolbox of DNA-based functional nanomachinery.
关键词： DNA origami,Reconfigurable nanostructure,Gold nanoparticle,Plasmonic nanostructure
更新于2025-09-23 15:19:57
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A DNA origami plasmonic sensor with environment-independent read-out
摘要： DNA origami is a promising technology for its reproducibility, flexibility, scalability and biocompatibility. Among the several potential applications, DNA origami has been proposed as a tool for drug delivery and as a contrast agent, since a conformational change upon specific target interaction may be used to release a drug or produce a physical signal, respectively. However, its conformation should be robust with respect to the properties of the medium in which either the recognition or the read-out take place, such as pressure, viscosity and any other unspecific interaction other than the desired target recognition. Here we report on the read-out robustness of a tetragonal DNA-origami/gold-nanoparticle hybrid structure able to change its configuration, which is transduced in a change of its plasmonic properties, upon interaction with a specific DNA target. We investigated its response when analyzed in three different media: aqueous solution, solid support and viscous gel. We show that, once a conformational variation is produced, it remains unaffected by the subsequent physical interactions with the environment.
关键词： molecular detection,DNA origami,gold nanoparticle,plasmonic sensor
更新于2025-09-19 17:13:59
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Localization microscopy at doubled precision with patterned illumination
摘要： MINFLUX offers a breakthrough in single molecule localization precision, but is limited in field of view. Here we combine centroid estimation and illumination pattern induced photon count variations in a conventional widefield imaging setup to extract position information over a typical micrometer-sized field of view. We show a near two-fold improvement in precision over standard localization with the same photon count on DNA-origami nanostructures and tubulin in cells, using DNA-PAINT and STORM imaging.
关键词： DNA-origami,DNA-PAINT,patterned illumination,tubulin,STORM,Localization microscopy
更新于2025-09-12 10:27:22
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Reconfigurable Plasmonic Diastereomers Assembled by DNA Origami
摘要： Herein, we reported self-assembled reconfigurable plasmonic diastereomers based on DNA nanotechnology. Up to three plasmonic chiral centers were organized by dynamic DNA origami platforms. Meanwhile, each chiral center could be individually controlled to switch between left-handed and right-handed states. Thus, complex and reconfigurable chiral plasmonic diastereomers with eight plasmonic stereoisomers were achieved, driven by programmed DNA reactions. With this plasmonic diastereomers, we demonstrated the existence of strong cross-talk near-filed coupling among chiral centers, and the coupling of chiral centers could substantially contribute to the overall CD signals. Our work provides an important bottom-up approach for building complex and dynamic chiral plasmonics and for probing the interactions of plasmonic chiral centers.
关键词： DNA origami,self-assembly,plasmonic chirality,chiral centers,diastereomers
更新于2025-09-12 10:27:22