Engineering DNA-based functional materials

Roh, Young Hoon; Ruiz, Roanna C. H.; Peng, Songming; Lee, Jong Bum; Luo, Dan

doi:10.1039/c1cs15162b

Cited by 268 publications

(192 citation statements)

References 82 publications

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“…We foresee that a large variety of topics in statistical physics can be experimentally addressed through the use of DNA supermolecules, including reentrant behaviors induced by competitive interactions (34,35), higher-order network-network critical points (36), and arrested states of matter (glasses and gels) (27). In the specific case of limited valence structures here discussed, our results set the basis to predict the thermal and kinetic stability of self-assembled DNA hydrogels (25), a finding with relevant implications in the design of commercial complex fluids with tailored properties. …”

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confidence: 99%

“…Because the binding between sticky overhangs is stronger than all other interparticle interactions (excluded volume, van der Waals, electrostatic), DNA nanostars provide an optimal model for highlighting the role of the valence. Similar DNA nanostars were studied by Luo and coworkers (24,25) to investigate their gelation in the presence of enzymatic catalysis. We operate in the absence of any enzymes to benefit the reversibility of the DNA interaction and systematically investigate the equilibrium phase behavior.…”

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confidence: 99%

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Phase behavior and critical activated dynamics of limited-valence DNA nanostars

Biffi

Cerbino

Bomboi

et al. 2013

Proc. Natl. Acad. Sci. U.S.A.

188

305

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Colloidal particles with directional interactions are key in the realization of new colloidal materials with possibly unconventional phase behaviors. Here we exploit DNA self-assembly to produce bulk quantities of "DNA stars" with three or four sticky terminals, mimicking molecules with controlled limited valence. Solutions of such molecules exhibit a consolution curve with an upper critical point, whose temperature and concentration decrease with the valence. Upon approaching the critical point from high temperature, the intensity of the scattered light diverges with a power law, whereas the intensity time autocorrelation functions show a surprising two-step relaxation, somehow reminiscent of glassy materials. The slow relaxation time exhibits an Arrhenius behavior with no signs of criticality, demonstrating a unique scenario where the critical slowing down of the concentration fluctuations is subordinate to the large lifetime of the DNA bonds, with relevant analogies to critical dynamics in polymer solutions. The combination of equilibrium and dynamic behavior of DNA nanostars demonstrates the potential of DNA molecules in diversifying the pathways toward collective properties and selfassembled materials, beyond the range of phenomena accessible with ordinary molecular fluids.DNA nanotechnology | limited valence colloids | critical behavior I n recent years, a strong effort has been devoted to introduce a new generation of micro-and nanocolloids interacting via strongly anisotropic forces. Anisotropic interactions can simply arise from a nonspherical particle shape or from more sophisticated physical and/or chemical patterning of the particle surface (1-7). An alternative strategy to produce complex nanoparticles is to exploit the self-assembly of DNA oligomers. The rational design of the DNA sequences enables guiding the association of multiple DNA strands into a rich variety of nanosized objects, such as geometrical figures, hollow capsules, and nanomachines, as well as more complex meso-and macroscopic structures (8-13). The selectivity of DNA binding can also be exploited to control the mutual interactions between the structures (14, 15), whereas the spontaneous assembly of DNA sequences enables producing large ensembles of particles. These properties make DNA a powerful tool to explore fundamental phenomena of soft matter and statistical physics, as indicated by previous studies of liquid-crystalline ordering and phase separations in solutions of short DNA oligomers (16-18). Here we exploit DNA self-assembly to experimentally address the phase behavior of particles interacting with specific valence, strength, and selectivity.Colloidal particles with controlled valence are the next step toward the realization of new colloidal materials and phases dependent on the presence of a small number of bonds (1-7). Theoretical and numerical studies (19) predict that a solution of low-valence particles should exhibit phase coexistence-the colloidal analog of the vapor-liquid coexistence in simple liquidsbut only at v...

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confidence: 99%

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confidence: 99%

Phase behavior and critical activated dynamics of limited-valence DNA nanostars

Biffi

Cerbino

Bomboi

et al. 2013

Proc. Natl. Acad. Sci. U.S.A.

188

305

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“…Hence, the cytoskeleton of liposomes should be constructed with defined and designable materials. To accomplish this aim, DNA nanotechnology, which uses limited components with high designability in a nanometer scale (11), is a feasible candidate to construct cytoskeleton structures in artificial cells.…”

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confidence: 99%

DNA cytoskeleton for stabilizing artificial cells

Kurokawa

Fujiwara

Morita

et al. 2017

Proc. Natl. Acad. Sci. U.S.A.

130

123

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Cell-sized liposomes and droplets coated with lipid layers have been used as platforms for understanding live cells, constructing artificial cells, and implementing functional biomedical tools such as biosensing platforms and drug delivery systems. However, these systems are very fragile, which results from the absence of cytoskeletons in these systems. Here, we construct an artificial cytoskeleton using DNA nanostructures. The designed DNA oligomers form a Y-shaped nanostructure and connect to each other with their complementary sticky ends to form networks. To undercoat lipid membranes with this DNA network, we used cationic lipids that attract negatively charged DNA. By encapsulating the DNA into the droplets, we successfully created a DNA shell underneath the membrane. The DNA shells increased interfacial tension, elastic modulus, and shear modulus of the droplet surface, consequently stabilizing the lipid droplets. Such drastic changes in stability were detected only when the DNA shell was in the gel phase. Furthermore, we demonstrate that liposomes with the DNA gel shell are substantially tolerant against outer osmotic shock. These results clearly show the DNA gel shell is a stabilizer of the lipid membrane akin to the cytoskeleton in live cells.iposomes have been used as artificial cell models to understand cell shape, membrane protein function, and lipid− protein interaction, among other biological functions (1-3). In addition, liposomes have been used as a platform for biosensing and as drug delivery systems (DDS) because of their excellent biocompatibility and biodegradability (4). However, liposomes collapse easily against environmental shifts and mechanical forces because of their low bending modulus. The fragility of liposomes causes uncontrolled leakage of the entrapped compounds and thus inhibits their use in biomedical applications and artificial cells experiments.In contrast, cell membranes are tolerant against environmental shifts and mechanical forces. The stability of cell membrane arises from the cytoskeleton underneath the membrane. The major component of cytoskeletons is actin (5). Actin gels show high elasticity (6), which ensures the stability of cell membranes against various forces. For liposomes, the use of actin filaments as a cytoskeleton is not an optimal strategy for the following three reasons: First, although actin bundles and actomyosin rings have been reconstituted in artificial cells (7,8), formation of an actin cortex underneath artificial membranes has been still challenging. Second, actin is hard to modify by chemical and genetic means because of its essentiality for cell growth. Third, the physicochemical properties of actin gels are still unclear (9, 10). Hence, the cytoskeleton of liposomes should be constructed with defined and designable materials. To accomplish this aim, DNA nanotechnology, which uses limited components with high designability in a nanometer scale (11), is a feasible candidate to construct cytoskeleton structures in artificial cells.DNA nanostructure...

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“…Exploiting the specificity of Watson-Crick base pairing has produced complex dynamic structures such as molecular computers,(1) motors,(2) nanoreactors,(3) as well as sensors and diagnostics. (4)(5)(6)(7)(8)(9)(10) More recently, the ability of certain drugs to intercalate within the DNA double helix and form strong physical complexes has been utilized to form physical prodrugs for cytotoxics. Farokhzad et al first demonstrated that a DNA aptamer could be loaded with doxorubicin (DOX), allowing targeted uptake into cells presenting the aptamer target.…”

Section: Introductionmentioning

confidence: 99%