Gels of DNA Nanostars Never Crystallize

Rovigatti, Lorenzo; Smallenburg, Frank; Romano, Flavio; Sciortino, Francesco

doi:10.1021/nn501138w

Cited by 78 publications

(122 citation statements)

References 50 publications

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“…40 The dynamics of both polyelectrolyte stars having inter-mediate number of arms and moderately polymer-grafted nanoparticles show sharp slowing down with increasing concentration that is symptomatic of incipient solidification. Sciortino and coworkers 105 have recently shown that nanoparticles with a moderate number of grafted DNA chains can form an equilibrium amorphous state in which the crystalline state is metastable. We expect the same situation to arise in soft star polyelectrolyte stars having a moderate number of arms.…”

Section: Discussionmentioning

confidence: 99%

Solution properties of star polyelectrolytes having a moderate number of arms

Chremos

Douglas

2017

The Journal of Chemical Physics

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We investigate polyelectrolyte stars having a moderate number of arms by molecular dynamics simulations of a coarse-grained model over a range of polyelectrolyte concentrations, where both the counter-ions and solvent are treated explicitly. This class of polymeric materials is found to exhibit rather distinct static and dynamic properties from linear and highly branched star polyelectrolyte solutions emphasized in past studies. Moderately branched polymers are particle-like in many of their properties, while at the same time they exhibit large fluctuations in size and shape as in the case of linear chain polymers. Correspondingly, these fluctuations suppress crystallization at high polymer concentrations, leading apparently to an amorphous rather than crystalline solid state at high polyelectrolyte concentrations. We quantify the onset of this transition by measuring the polymer size and shape fluctuations of our model star polyelectrolytes and the static and dynamic structure factor of these solutions over a wide range of polyelectrolyte concentration. Our findings for star polyelectrolytes are similar to those of polymer-grafted nanoparticles having a moderate grafting density, which is natural given the soft and highly deformable nature of both of these ‘particles’.

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Section: Discussionmentioning

confidence: 99%

Solution properties of star polyelectrolytes having a moderate number of arms

Chremos

Douglas

2017

The Journal of Chemical Physics

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“…191 In particular, it was shown that patchy systems combining low valence, bond flexibility and soft interactions can stabilize the liquid phase in contrast to the solid one even in the zero-temperature limit, meaning that even at extremely low temperatures the entropic term prevails over the energetic term in the free energy balance of such systems. 190 These results were found for patchy models apt to describe associating fluids or DNA-coated colloids with limited valence, but also tetravalent DNA nanostars, i.e.…”

Section: Patchy Particles From the Bottom-up Routementioning

confidence: 99%

“…extremely flexible patchy units with four bonding patches, were shown to never crystallize and form instead a thermodynamically stable, fully bonded equilibrium gel. 191 In recent years, polymer-based macromolecules or nanocomposites (such as mixtures of polymers and colloids) were shown to be extremely powerful and versatile systems for the self-assembly of soft functionalized nanoparticles. 26 Janus-like, triblock, striped and multi-patch units can indeed be created by playing with the topology, the geometry and the type of polymeric macromolecules.…”

Section: Patchy Particles From the Bottom-up Routementioning

confidence: 99%

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Limiting the valence: advancements and new perspectives on patchy colloids, soft functionalized nanoparticles and biomolecules

Bianchi

Capone

Coluzza

et al. 2017

Phys. Chem. Chem. Phys.

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Limited bonding valence, usually accompanied by well-defined directional interactions and selective bonding mechanisms, is nowadays considered among the key ingredients to create complex structures with tailored properties: even though isotropically interacting units already guarantee access to a vast range of functional materials, anisotropic interactions can provide extra instructions to steer the assembly of specific architectures. The anisotropy of effective interactions gives rise to a wealth of self-assembled structures both in the realm of suitably synthesized nano-and micro-sized building blocks and in nature, where the isotropy of interactions is often a zero-th order description of the complicated reality.In this review, we span a vast range of systems characterized by limited bonding valence, from patchy colloids of new generation to polymer-based functionalized nanoparticles, DNA-based systems and proteins, and describe how the interaction patterns of the single building blocks can be designed to tailor the properties of the target final structures.

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“…This treatment is sufficient to obtain good agreement with experimental data on the structural, mechanical, and especially the thermodynamic properties of single-and double-stranded DNA. Consequently, the model has provided key insights into many different processes relevant to DNA nanotechnology [32][33][34][35][36][37][38][39][40] and biophysics [41][42][43][44][45] and importantly has also been shown to provide direct agreement with experimentally measured properties on a range of systems including DNA overstretching, 45 a two-footed DNA walker, 35 and toehold-mediated strand displacement. 39,46 Despite these achievements, there are some areas where oxDNA can be improved.…”

Section: Introductionmentioning

confidence: 99%

Introducing improved structural properties and salt dependence into a coarse-grained model of DNA

Snodin

Randisi

Mosayebi

et al. 2015

The Journal of Chemical Physics

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444

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We introduce an extended version of oxDNA, a coarse-grained model of deoxyribonucleic acid (DNA) designed to capture the thermodynamic, structural, and mechanical properties of single-and double-stranded DNA. By including explicit major and minor grooves and by slightly modifying the coaxial stacking and backbone-backbone interactions, we improve the ability of the model to treat large (kilobase-pair) structures, such as DNA origami, which are sensitive to these geometric features. Further, we extend the model, which was previously parameterised to just one salt concentration ([Na + ] = 0.5M), so that it can be used for a range of salt concentrations including those corresponding to physiological conditions. Finally, we use new experimental data to parameterise the oxDNA potential so that consecutive adenine bases stack with a different strength to consecutive thymine bases, a feature which allows a more accurate treatment of systems where the flexibility of single-stranded regions is important. We illustrate the new possibilities opened up by the updated model, oxDNA2, by presenting results from simulations of the structure of large DNA objects and by using the model to investigate some salt-dependent properties of DNA. C 2015 AIP Publishing LLC. [http://dx

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Gels of DNA Nanostars Never Crystallize

Cited by 78 publications

References 50 publications

Solution properties of star polyelectrolytes having a moderate number of arms

Solution properties of star polyelectrolytes having a moderate number of arms

Limiting the valence: advancements and new perspectives on patchy colloids, soft functionalized nanoparticles and biomolecules

Introducing improved structural properties and salt dependence into a coarse-grained model of DNA

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