Volume and porosity thermal regulation in lipid mesophases by coupling mobile ligands to soft membranes

Parolini, Lucia; Mognetti, Bortolo Matteo; Kotar, Jurij; Eiser, Erika; Cicuta, Pietro; Michele, Lorenzo Di

doi:10.1038/ncomms6948

Cited by 104 publications

(218 citation statements)

References 54 publications

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“…For example, in asymmetric binary mixtures of mDNACCs, more open structures are expected, especially when nonspecific repulsions are introduced [17], of which the self-assembly mechanism can be very different from that of conventional patchy particle systems [30,31,34]. Moreover, in experimental systems of mobile DNA coated liposomes, the combination of vibrational entropy and deformability are expected leading to the formation of more interesting structures [35][36][37][38]. Additionally, the method developed for the infinite binding strength limit could also be modified to simulate other network systems, e.g.…”

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confidence: 99%

Entropy Stabilizes Floppy Crystals of Mobile DNA-Coated Colloids

Ruiz

2018

Phys. Rev. Lett.

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Grafting linkers with open ends of complementary single-stranded DNA makes a flexible tool to tune interactions between colloids, which facilitates the design of complex self-assembly structures. Recently, it has been proposed to coat colloids with mobile DNA linkers, which alleviates kinetic barriers without high-density grafting, and also allows the design of valency without patches. However, the self-assembly mechanism of this novel system is poorly understood. Using a combination of theory and simulation, we obtain phase diagrams for the system in both two and three dimensional spaces, and find stable floppy square and CsCl crystals when the binding strength is strong, even in the infinite binding strength limit. We demonstrate that these floppy phases are stabilized by vibrational entropy, and "floppy" modes play an important role in stabilizing the floppy phases for the infinite binding strength limit. This special entropic effect in the self-assembly of mobile DNA-coated colloids is very different from conventional molecular self-assembly, and it offers new axis to help design novel functional materials using mobile DNA-coated colloids.Nucleic acids are ubiquitous in nature because of their capability of encoding large amounts of information via canonical Watson-Crick base-paring interactions [1]. With the help of chemical methods to make synthetic oligonucleotides of arbitrary sequences, one can use specific binding interactions between single-stranded DNA (ssDNA) chains to program selective interactions between different colloidal particles. For example, one can graft DNA linkers to the surface of colloidal particles with open ends of ssDNAs. These ssDNA tails serve as "sticky ends" that bind specifically to other colloids coated with ssDNA tails of complementary sequence, which offers a novel way of manipulating the self-assembly of colloidal particles [2,3]. By using DNA-coated colloids (DNACCs), a number of ordered crystals [4-10] and selfassembled "colloidal molecules" [11] have been obtained in experiments, while the self-assembly mechanism of DNACCs is still not well understood [9,12,13]. For example, the diffusionless transformation from a floppy crystal to the other compact crystal has been observed in experimental systems while the underlying mechanism remains not fully resolved [13].Recently, a novel system of mobile DNA-coated colloids (mDNACCs) was introduced that displays qualitatively new properties [14,15]. Compared with immobile DNA-coated colloidal systems, mDNACCs have a broader temperature window for self-assembly, and therefore allow the better control over the assembly process [14]. Mobility of DNA linkers also allows particles to more easily roll around each other and rearrange [14,16], without grafting of very high density. Moreover, unlike colloids with patches in specific locations [11,16], the interaction in mDNACCs is intrinsically a many-body potential, which could be employed to control the "valency" of particles without patches by tuning nonspecific repulsions between the p...

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confidence: 99%

Entropy Stabilizes Floppy Crystals of Mobile DNA-Coated Colloids

Ruiz

2018

Phys. Rev. Lett.

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“…[10] Since Brownian motion rarely results in interliposomal distances below 5-10 nm, [11] geometry suggests that short LiNAduplexes (e.g. Thec ooperative action of LiNA duplexes deforms docked liposomes,w hile increasing the double-bilayer contact area.…”

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A DNA‐Programmed Liposome Fusion Cascade

et al. 2017

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Chemically engineered and functionalized nanoscale compartments are used in bottom-up synthetic biology to construct compartmentalized chemical processes. Progressively more complex designs demand spatial and temporal control over entrapped species. Here, we address this demand with a DNA-encoded design for the successive fusion of multiple liposome populations. Three individual stages of fusion are induced by orthogonally hybridizing sets of membrane-anchored oligonucleotides. Each fusion event leads to efficient content mixing and transfer of the recognition unit for the subsequent stage. In contrast to fusion-protein-dependent eukaryotic vesicle processing, this artificial fusion cascade exploits the versatile encoding potential of DNA hybridization and is generally applicable to small and giant unilamellar vesicles. This platform could thus enable numerous applications in artificial cellular systems and liposome-based synthetic pathways.

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“…1), the complexation free energy ∆G i 1 , ...,i m 28 also includes rotational and translational entropic costs controlled by the length of the spacers and by the size of the particles. 7 Using Eq. (6) in Eq.…”

Section: Free Energy Calculationmentioning

confidence: 99%

“…[3][4][5][6][7][8][9][10][11] Many functionalization schemes rely on one-to-one ligand-receptor interactions, but recently, designs featuring multi-linker complexation have been proposed to extend the accessible range of functionalities. 9,[12][13][14][15] In particular, Parolini et al 13 adopted three-linker complexes enabling toehold-mediated strand exchange reactions 16 to control aggregation kinetics of lipid vesicles coated with DNA linkers.…”

Section: Introductionmentioning

confidence: 99%

Communication: Free energy of ligand-receptor systems forming multimeric complexes

Michele

Bachmann

Parolini

et al. 2016

The Journal of Chemical Physics

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Ligand-receptor interactions are ubiquitous in biology and have become popular in materials in view of their applications to programmable self-assembly. Although complex functionalities often emerge from the simultaneous interaction of more than just two linker molecules, state of the art theoretical frameworks enable the calculation of the free energy only in systems featuring one-to-one ligand/receptor binding. In this Communication, we derive a general formula to calculate the free energy of systems featuring simultaneous direct interaction between an arbitrary number of linkers. To exemplify the potential and generality of our approach, we apply it to the systems recently introduced by Parolini et al. [ACS Nano 10, 2392

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Volume and porosity thermal regulation in lipid mesophases by coupling mobile ligands to soft membranes

Cited by 104 publications

References 54 publications

Entropy Stabilizes Floppy Crystals of Mobile DNA-Coated Colloids

Entropy Stabilizes Floppy Crystals of Mobile DNA-Coated Colloids

A DNA‐Programmed Liposome Fusion Cascade

Communication: Free energy of ligand-receptor systems forming multimeric complexes

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