Kinetic control of the coverage of oil droplets by DNA-functionalized colloids

Joshi, Darshana; Bargteil, Dylan; Caciagli, Alessio; Burelbach, Jérôme; Xing, Zhongyang; Nunes, André S.; Pinto, Diogo; Araújo, Nuno A. M.; Brujić, Jasna; Eiser, Erika

doi:10.1126/sciadv.1600881

Cited by 54 publications

(58 citation statements)

References 42 publications

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“…DNA has also been used as a scaffold or linker to assemble secondary components including proteins, gold nanoparticles and liposomes . In addition, networks of emulsion droplets or colloid‐coated droplets have been created using DNA linkers. Yet in all cases, the linkage was based on biotinylated DNA, which requires additional efforts to graft streptavidin onto the droplet surface.…”

Section: Introductionmentioning

confidence: 99%

Programmable Functionalization of Surfactant‐Stabilized Microfluidic Droplets via DNA‐Tags

Jahnke

Weiss

Frey

et al. 2019

Adv Funct Materials

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Droplet-based microfluidics has emerged as a powerful tool in synthetic biology. For many applications, chemical functionalization of the droplets is a key process. Therefore, a straightforward and broadly applicable approach is developed to functionalize the inner periphery of microfluidic droplets with diverse reactive groups and components. Instead of covalent modification of the droplet-stabilizing surfactants, this method relies on cholesteroltagged DNA that self-assembles at the droplet periphery. The cholesteroltagged DNA serves as an attachment handle for the recruitment of complementary DNA. The complementary DNA can carry diverse functional groups. We exemplify our method by demonstrating the attachment of amine groups, DNA nanostructures, microspheres, a minimal actin cortex, and leukemia cells to the droplet periphery. It is further shown that the DNAmediated attachment to the droplet periphery is temperature-responsive and reversible. It is envisioned that droplet functionalization via DNA handles will help to tailor droplet interfaces for diverse applications-featuring programmable assembly, unique addressability, and stimuli-responsiveness.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adfm.201808647. not universally applicable-it depends on the success of the chemical synthesis and can interfere with the stability and the physical properties of the droplets. Moreover, the binding of the functional group to the droplet periphery is irreversible.DNA nanotechnology, [12] on the other hand can attain the programmable assembly of arbitrary nanoscale architectures like DNA-based lattices, [13] nanopores, [14][15][16] or lid-containing boxes. [17,18] DNA has also been used as a scaffold or linker to assemble secondary components including proteins, [19] gold nanoparticles [20] and liposomes. [21] In addition, networks of emulsion droplets [22,23] or colloid-coated droplets [24] have been created using DNA linkers. Yet in all cases, the linkage was based on biotinylated DNA, which requires additional efforts to graft streptavidin onto the droplet surface. Furthermore, it has never been demonstrated that it is possible to functionalize the interior of block-copolymer surfactantstabilized droplets with DNA.Here, we present a broadly applicable method for functionalizing microfluidic droplets utilizing the hydrophobic interaction of cholesterol-tagged DNA with the droplet-stabilizing surfactant. Notably, the interaction of cholesterol with perfluorinated chains has never been described or exploited before. We show that DNA handles can serve as reversible anchoring points for various components including reactive groups, DNA nanostructures, beads, proteins or even cells. The use of off-the-shelf available DNA holds considerable advantages compared to standard methods for droplet functionalization, including: the broad scope of options for site-directed chemical functionalization, the addressability and programmability due to specific base pairin...

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Section: Introductionmentioning

confidence: 99%

Programmable Functionalization of Surfactant‐Stabilized Microfluidic Droplets via DNA‐Tags

Jahnke

Weiss

Frey

et al. 2019

Adv Funct Materials

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“…Such proposals rely on self-assembly through tunable enthalpic and entropic interactions guiding the system toward thermodynamic equilibrium. In addition, introducing mobile linkers to colloids 15 , liposomes 16 , 17 , and droplets 18 – 20 avoids kinetic traps along the self-assembly pathways. However, the design principle that invokes sequential self or directed assembly has not yet been addressed due to the absence of an underlying technology.…”

Section: Introductionmentioning

confidence: 99%

Sequential self-assembly of DNA functionalized droplets

et al. 2017

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Complex structures and devices, both natural and manmade, are often constructed sequentially. From crystallization to embryogenesis, a nucleus or seed is formed and built upon. Sequential assembly allows for initiation, signaling, and logical programming, which are necessary for making enclosed, hierarchical structures. Although biology relies on such schemes, they have not been available in materials science. Here, we demonstrate programmed sequential self-assembly of DNA functionalized emulsions. The droplets are initially inert because the grafted DNA strands are pre-hybridized in pairs. Active strands on initiator droplets then displace one of the paired strands and thus release its complement, which in turn activates the next droplet in the sequence, akin to living polymerization. Our strategy provides time and logic control during the self-assembly process, and offers a new perspective on the synthesis of materials.

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“…Several protocols and techniques have been developed for the design of complex 2D4,5 and 3D6–8 geometries and networks. The binding specificity and programmability of the DNA nucleotides, together with the continuous reduction in the costs of production of synthetic DNA, permit design of DNA sequences programmed to self-assemble in bulk quantities of desired nanostructures with controlled binding properties and tuneable response to external phenomena such as pH,9 temperature,10 or light 11,12. Along these lines, beside being thoroughly investigated in single-molecule studies,13–15 DNA has been also successfully applied to investigate the kinetic control of oil droplet functionalized colloids,11 to drive the assembly of nanoparticles into macroscopic materials,16 to organize nanocrystal molecules,17 and to guide the crystallization of colloidal nanoparticles 18.…”

Section: Introductionmentioning

confidence: 99%

“…The binding specificity and programmability of the DNA nucleotides, together with the continuous reduction in the costs of production of synthetic DNA, permit design of DNA sequences programmed to self-assemble in bulk quantities of desired nanostructures with controlled binding properties and tuneable response to external phenomena such as pH,9 temperature,10 or light 11,12. Along these lines, beside being thoroughly investigated in single-molecule studies,13–15 DNA has been also successfully applied to investigate the kinetic control of oil droplet functionalized colloids,11 to drive the assembly of nanoparticles into macroscopic materials,16 to organize nanocrystal molecules,17 and to guide the crystallization of colloidal nanoparticles 18. In addition, the hydrophilic character of DNA is exploited for the formation of 3D networks19,20 able to hold large amounts of water, similar to polymeric hydrogels,21 a property of major interest for the development of drug delivery, sensing, and tissue engineering applications 20…”

Section: Introductionmentioning

confidence: 99%

Microrheology of DNA hydrogel gelling and melting on cooling

et al. 2018

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We present systematic characterisation by means of dynamic light scattering and particle tracking techniques of the viscosity and of the linear viscoelastic moduli, G'(ω) and G''(ω), for two different DNA hydrogels. These thermoreversible systems are composed of tetravalent DNA-made nanostars whose sticky sequence is designed to provide controlled interparticle bonding. While the first system forms a gel on cooling, the second one has been programmed to behave as a re-entrant gel, turning again to a fluid solution at low temperature. The frequency-dependent viscous and storage moduli and the viscosity reveal the different viscoelastic behavior of the two DNA hydrogels. Our results show how little variations in the design of the DNA sequences allow tuning of the mechanical response of these biocompatible all-DNA materials.

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Kinetic control of the coverage of oil droplets by DNA-functionalized colloids

Abstract: Controlled adsorption and phase behavior of colloids at liquid interface.

Cited by 54 publications

References 42 publications

Programmable Functionalization of Surfactant‐Stabilized Microfluidic Droplets via DNA‐Tags

Programmable Functionalization of Surfactant‐Stabilized Microfluidic Droplets via DNA‐Tags

Sequential self-assembly of DNA functionalized droplets

Microrheology of DNA hydrogel gelling and melting on cooling

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