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At least 19 recordsLinked to original sources
PubMed2006

A study of DNA tube formation mechanisms using 4-, 8-, and 12-helix DNA nanostructures.

This paper describes the design and characterization of a new family of rectangular-shaped DNA nanostructures (DNA tiles) containing 4, 8, and 12 helices. The self-assembled morphologies of the three tiles were also investigated. The motivation for designing this set of DNA nanostructures originated from the desire to produce DNA lattices containing periodic cavities of programmable dimensions and to investigate the mechanism of DNA tube formation. Nine assembly scenarios have been investigated through the combination of the three different tiles and three sticky end association strategies. Imaging by atomic force microscopy (AFM) revealed self-assembled structures with varied cavity sizes, lattice morphologies, and orientations. Six samples show only tube formation, two samples show both 2D lattices (>2 microm) and tubes, and one sample shows only 2D lattices without tubes. We found that a lower tile dimensional anisotropy, weaker connection, and corrugated design favor the large 2D array formation, while the opposite (higher tile anisotropy, stronger connection, and uncorrugated design) favors tube formation. We discuss these observations in terms of an energy balance at equilibrium and the kinetic competition between diffusion-limited lateral lattice growth versus fluctuation of the lattice to form tubes at an early stage of the assembly. The DNA nanostructures and their self-assembly demonstrated herein not only provide a new repertoire of scaffolds to template the organization of nanoscale materials, but may also provide useful information for investigating other self-assembly systems.

Anisotropy↗
PubMed2026

Insertion of CG repeats and 3' terminus overhangs drive B-to-Z transition: A case study with NF-κB bearing DNA nanostructures.

Z-DNA, a non-canonical helical structure of DNA plays a vital role in various biological processes, including transcription and genomic stability. Though low concentration of trivalent cations is known to induce B-Z transition, the effect of short CG repeats, overhangs sequences, loop length and order of nucleotides on Z-DNA formation in larger DNA is utterly unknown. Earlier, a series of self-assembled branched DNA (bDNA) nanostructures having 5T in the loop are reported to be resistant to B-to-Z DNA transition irrespective of the overhang sequences. Since the presence of alternative purine/pyrimidine sequences and direction of oligonucleotides play a vital role during replication and transcription, we hypothesize that the insertion of a small number of CG repeats, or a change in direction of overhang sequences may influence the B-to-Z DNA transition. Here, we show that Z-DNA formation was induced by inserting CG repeats into bDNA structures that were previously resistant to B-Z transition. Moreover, B-Z transition was also observed when overhangs were introduced at the 3' terminus. The generality of the approach of B-Z transition was demonstrated in a series of bDNA structures including the bDNA having NF-kβ sequences. Different dye binding experiments suggest the formation of Z-DNA in bDNA having overhangs at the 3' terminus against the control of bDNA with 5' overhangs. Interestingly, the melting temperature (Tm) was substantially reduced to 55 °C in the Z-DNA as compared to the LaCl3-induced condensed DNA having Tm of 77 °C. Fluorescence study also supports the presence of minor groove in Z-DNA which binds Hoechst. ITC indicates an entropy- and enthalpy-driven favorable binding between lanthanide cations and bDNA. Thus, the present study establishes a synthetic bDNA nanotechnology platform for systematically investigating how local sequence architecture, including the insertion of CG repeats, loop length, and overhang orientation influences B-to-Z conformational switching under controlled experimental conditions.

B-Z transition↗
PubMed2025

DNA Nanostructure Self-Assembly in an Aqueous Ionic Liquid Solution with Enhanced Stability and Target Binding Affinity.

DNA nanostructure-enabled functional constructs have shown potential to improve healthcare outcomes by offering advanced disease diagnostic and therapeutic strategies. Translating this potential of DNA nanostructure-based constructs to real life applications relies on maintaining and enhancing the structural integrity and functions of the surface-anchored moieties. In this study, we explored the possibility of utilizing choline dihydrogen phosphate (CDHP) solution, an aqueous solution of ionic liquid, to assemble DNA nanostructures of different sizes and complexities with enhanced biostability and ligand binding affinity. We show successful formation of the DNA nanostructures in aqueous CDHP solution using gel electrophoresis, atomic force microscopy (AFM), and circular dichroism (CD). Biostability assays reveal that the aqueous CDHP solution may provide passive protection to DNA nanostructures against DNase I and human serum for up to 48 h. We also demonstrate that this enhanced biostability arises both from the structural conformation imparted during CDHP-mediated folding and from the presence of free CDHP ions in the solution. Notably, removal of free ions reduced the passive protection effect, but did not eliminate it, indicating the contribution of both folding and surrounding free ions. Using flow cytometry and surface plasmon resonance assays, we show that the presence of aqueous CDHP solution can enhance the binding of aptamer-functionalized DNA nanostructures to specific receptors on acute myeloid leukemia (AML) cells. Our strategy of using ionic liquid solution for one-pot preparation with enhanced stability and functionality offers a robust, simpler and faster alternative for DNA nanostructure-based constructs.

Ionic Liquids↗
PubMed2006

Combinatorial self-assembly of DNA nanostructures.

Here we report a modular design of self-assembly of DNA nanostructures in a combinatorial approach; a square with approximately 25 nm cavity dimension, a chair with approximately 80 nm in height and a line with approximately 100 nm in length are formed through combinations of four cross-shaped DNA tiles which are kept constant and six variable linker tiles.

DNA↗
PubMed2005

Enzymatic fabrication of DNA nanostructures: extension of a self-assembled oligonucleotide monolayer on gold arrays.

Nucleic acid nanostructures are useful as templates for bionanofabrication of composite molecular nanostructures in materials science, molecular electronics, and biosensing. Here, we demonstrate that terminal deoxynucleotidyl transferase, which repetitively adds mononucleotides to the 3' end of a short DNA initiator, can be used to rapidly fabricate DNA nanostructures up to 121 nm high with lateral dimensions from 0.1 to 4 mum in 2 h. These programmable scaffolds can potentially be employed to build more complex nanostructures consisting of natural or unnatural nucleotides with selective docking sites along the single-stranded DNA.

DNA↗
PubMed2006

Mastering the complexity of DNA nanostructures.

The self-assembly of oligodeoxynucleotides is a versatile and powerful tool for the construction of objects in the nanoscale. The strictly information-driven pairing of DNA fragments can be used to rationally design and build nanostructures with planned topologies and geometries. Taking advantage of the steadily expanding library of well-characterized DNA motifs, several examples of structures with different dimensionalities have appeared in the literature in the past few years, laying the foundations for a promising DNA-mediated, bottom-up approach to nanotechnology. This article focuses on recent developments in this area of research and proposes a classification of DNA nanostructures based on topological considerations in addition to describing strategies for tackling the inherent complexities of such an endeavor.

Binding Sites↗
PubMed2005

Nanostructured DNA templates.

We have developed methods for nanostructure fabrication relying on the size and shape of a polynucleotide to dictate the overall structure of an assemblage of individual semiconductor nanoparticles. Use of the circular plasmids pUCLeu4 and phi chi 174 when anchored to a suitably derivatized substrate yields arrays of semiconductor nanoparticles matching the shapes of the biopolymer stabilizer. The viability of the methodology was confirmed using high-resolution transmission electron microscopy and selected-area electron diffraction.

Nanostructures↗
PubMed2006

Characterization and modulation of the hierarchical self-assembly of nanostructured DNA tiles into supramolecular polymers.

We present a set of DNA supramolecular architectures based on the polymerization of discrete DNA tiles having the shape of parallelograms and designed to have a one-dimensional inter-tile connectivity. Tiles bind to each other with two connections, which have different thermal stabilities. We discuss how this difference in stability implies that the same monomeric tile can yield supramolecular polymers of different shapes just by changing the polymerization conditions. We show how this system reacts to external stimuli by interconverting between some of its possible states. Concurrently, we show how performing the polymerization on a surface can influence its outcome.

Base Sequence↗
PubMed1995

A new DNA nanostructure, the G-wire, imaged by scanning probe microscopy.

G-DNA is a polymorphic family of quadruple helical nucleic acid structures containing guanine tetrad motifs [G-quartets; Williamson, J.R., Raghuraman, M.K. and Cech, T.R. (1989) Cell 59, 871-880; Williamson, J.R. (1993) Proc. Natl. Acad. Sci. USA 90, 3124-3124]. Guanine rich oligonucleotides that are self-complimentary, as found in many telomeric G-strand repeat sequences, form G-DNA in the presence of monovalent and/or divalent metal cations. In this report we use the atomic force microscope (AFM) to explore the structural characteristics of long, linear polymers formed by the telomeric oligonucleotide d(GGGGTTGGGG) in the presence of specific metal cations. In the AFM these polymers, termed G-wires, appear as filaments whose height and length are determined by the metal ions present during the self-assembly process. The highly ordered, controllable self-assembly of G-wires could provide a basis for developing advanced biomaterials.

Base Sequence↗
PubMed2006

Atomic-level simulations of seeman DNA nanostructures: the paranemic crossover in salt solution.

We use molecular dynamics (MD) simulations to understand the structure and stability of various paranemic crossover (PX) DNA molecules, synthesized recently by Seeman and co-workers at New York University. These studies include all atoms of the PX structures with an explicit description of solvent and ions. The average dynamics structures over the last 1 ns of the 3-ns simulation preserve the Watson-Crick hydrogen bonding as well as the helical structure. The root mean-square deviation in coordinates with respect to the MD averaged structure converges to 2-3 A for PX55, PX65, and PX85, but for PX75 and PX95 the root mean-square deviation in coordinates exhibits large fluctuations, indicating an intrinsic instability. The PX structures are structurally more rigid compared to the canonical B-DNA without crossover. We have developed a strain energy analysis method based on the nearest-neighbor interaction and computed the strain energy for the PX molecules compared to the B-DNA molecules of the same length and sequence. PX65 has the lowest calculated strain energy (approximately -0.77 kcal/mol/bp), and the strain increases dramatically for PX75, PX85, and PX95. PX55 has the highest strain energy (approximately 1.85 kcal/mol/bp) making it unstable, which is in accordance with the experimental results. We find that PX65 has helical twist and other helical structural parameters close to the values for normal B-DNA of similar length and sequence. Vibrational mode analysis shows that compared to other PX motifs, PX65 has the smallest population of the low-frequency modes that are dominant contributors for the conformational entropy of the PX DNA structures. All these results indicate that PX65 is structurally more stable compared to other PX motifs, in agreement with experiments. These results should aid in designing optimized DNA structures for use in nanoscale components and devices.

Computer Simulation↗
PubMed2006

The architectonics of programmable RNA and DNA nanostructures.

The past several years have witnessed the emergence of a new world of nucleic-acid-based architectures with highly predictable and programmable self-assembly properties. For almost two decades, DNA has been the primary material for nucleic acid nanoconstruction. More recently, the dramatic increase in RNA structural information led to the development of RNA architectonics, the scientific study of the principles of RNA architecture with the aim of constructing RNA nanostructures of any arbitrary size and shape. The remarkable modularity and the distinct but complementary nature of RNA and DNA nanomaterials are revealed by the various self-assembly strategies that aim to achieve control of the arrangement of matter at a nanoscale level.

Base Sequence↗
PubMed2003

Oriented and vectorial immobilization of linear M13 dsDNA between interdigitated electrodes--towards single molecule DNA nanostructures.

The ability to control molecules at a resolution well below that offered by photolithography has gained much interest recently. DNA is a promising candidate for this task since it offers excellent specificity in base-pairing combined with addressability at the nanometer scale. New applications in biosensing, e.g. interaction analysis at the single molecule level, or nanobiotechnology, e.g. ultradense DNA microarrays, have been devised that rely on stretched DNA bridges. The basic technology required is the ability to deposit spatially defined, stretched DNA-bridges between anchoring structures on surfaces. In this paper we present two techniques for spanning 2 microm long dsDNA bridges between neighboring interdigitated electrodes (IDEs). The extended DNA used was linearized M13 dsDNA (M13mp18 7231 bp, ca. 2.5 microm length), either unmodified, or with chemical modifications at both ends. The first approach is based on the dielectrophoretic (DEP) concentration and alignment of linearized wild-type dsDNA. IDEs with 1.7 microm spacing are driven with an AC voltage around 1 MHz leading to field strengths in the order of 1 MV m(-1). The dsDNA is polarized and linearized by the force field and accumulates in the gap between two neighboring electrodes. This process is reversible and was visualized by fluorescence staining of M13 DNA using PicoGreen, as intercalating dye. The resulting dsDNA bridges and their orientation are discernible under the fluorescence microscope using fluorescent particles of different color. The particles are tagged with sequence specific peptide nucleic acid (PNA) probes that bind to the DNA double strand at specific sites. The second approach is based on asymmetric electrochemical modification of a gold IDE with 2.0 microm spacings followed by spontaneous or stimulated deposition of a chemically modified M13-DNA. One side of the IDE was selectively coated with streptavidin by electropolymerization of a novel hydrophilic conductive polymer in the presence of the binding protein. The second side was modified with gold nanoparticles by reductive plating from aqueous gold chloride solution. An asymmetric double stranded (ds) M13 DNA carrying a 5'-thiol group at one end and a 5'-biotin at the other end was obtained by polymerase chain reaction (PCR) using two differently labeled primers. For DNA bridges to form spontaneously the modified IDE was incubated over night with a 50 nM solution of the modified M13 DNA. Potential applications of DNA-bridge formation in biosensing and biotechnology are discussed.

Adsorption↗