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Erika Eiser

Publications and source records attributed to Erika Eiser.

34 records · Page 2Linked to original sources
arXiv2018

Inducing transparency in the films of highly scattering particles

Today colloids are employed in various products from creams and coatings to electronics. The ability to control their chemical, optical, or electronic features by controlling their size and shape explains why these materials are so widely employed. Nevertheless, altering some of these properties may also lead to some undesired side effects, one of which is an increase in optical scattering upon concentration. Here, we address this strong scattering issue in films made of colloids with high surface roughness. We focus on raspberry type polymeric particles made of a spherical polystyrene core decorated by small hemispherical domains of acrylate. Owing to their surface charge and model roughness, aqueous dispersions of these particles display an unusual stability against aggregation. Under certain angles, their solid films display a brilliant red color due to Bragg scattering but otherwise appear completely white on account of`strong scattering. To suppress the scattering and induce transparency, we prepared films by hybridizing them either with oppositely-charged PS-particles that fit the length-scale of the raspberry roughness or with quantum dots. We report that the smaller PS-particles prevent raspberry particle aggregation in solid films and suppress scattering by decreasing the spatial variation of the refractive index. We believe that the results presented here provide a simple strategy to suppress strong scattering of rough particles and allow for their utilization in optical coatings, cosmetics, or photonics.

physics.app-ph↗
arXiv2017

Microrheology of DNA Hydrogels

A key objective in DNA-based material science is understanding and precisely controlling the mechanical properties of DNA hydrogels. We perform microrheology measurements using diffusing-wave spectroscopy (DWS) to investigate the viscoelastic behavior of a hydrogel made of Y-shaped DNA nano-stars over a wide range of frequencies and temperatures. Results show a clear liquid-to-equilibrium-gel transition as the temperature cycles up and down across the melting-temperature region for which the Y-DNA bind to each other. These first measurements reveal the crossover of the elastic G'(ω) and loss modulus G'(ω) when the DNA-hydrogel formed at low temperatures is heated to a fluid phase of DNA nano-stars well above the melt temperature Tm. We show that the crossover relates to the life-time of the DNA-bond and also that percolation coincides with the systems' Tm. The approach demonstrated here can be easily extended to more complicated DNA hydrogel systems and provides guidance for the future design of such transient, semi-flexible networks that can be adapted to the application of molecular sensing and controlled release.

cond-mat.soft↗
arXiv2017

A Unified Description of Colloidal Thermophoresis

We use the dynamic length and time scale separation in suspensions to formulate a general description of colloidal thermophoresis. Our approach allows an unambiguous definition of separate contributions to the colloidal flux and clarifies the physical mechanisms behind non-equilibrium motion of colloids. In particular, we derive an expression for the interfacial force density that drives single-particle thermophoresis in non-ideal fluids. The issuing relations for the transport coefficients explicitly show that interfacial thermophoresis has a hydrodynamic character that cannot be explained by a purely thermodynamic consideration. Our treatment generalises the results from other existing approaches, giving them a clear interpretation within the framework of non-equilibrium thermodynamics.

cond-mat.soft↗
arXiv2017

DNA-coated Functional Oil Droplets

Many industrial soft materials often include oil-in-water (O/W) emulsions at the core of their formulations. By using tuneable interface stabilizing agents, such emulsions can self-assemble into complex structures. DNA has been used for decades as a thermoresponsive highly specific binding agent between hard and, recently, soft colloids. Up until now, emulsion droplets functionalized with DNA had relatively low coating densities and were expensive to scale up. Here a general O/W DNA-coating method using functional non-ionic amphiphilic block copolymers, both diblock and triblock, is presented. The hydrophilic polyethylene glycol ends of the surfactants are functionalized with azides, allowing for efficient, dense and controlled coupling of dibenzocyclooctane functionalized DNA to the polymers through a strain-promoted alkyne-azide click reaction. The protocol is readily scalable due to the triblock's commercial availability. Different production methods (ultrasonication, microfluidics and membrane emulsification) are used with different oils (hexadecane and silicone oil) to produce functional droplets in various size ranges (sub-micron, $\sim 20\,\mathrm{μm}$ and $> 50\,\mathrm{μm}$), showcasing the generality of the protocol. Thermoreversible sub-micron emulsion gels, hierarchical "raspberry" droplets and controlled droplet release from a flat DNA-coated surface are demonstrated. The emulsion stability and polydispersity is evaluated using dynamic light scattering and optical microscopy. The generality and simplicity of the method opens up new applications in soft matter and biotechnological research and industrial advances.

cond-mat.soft↗
arXiv2017

Liquid crystalline behaviour of self-assembled Laponite PLL-PEG nanocomposites

Synthetic Laponite-clay particles with platelet-like shape display strong aging when dispersed in aqueous solutions, preventing latter from reaching their natural liquid-crystalline equilibrium state. Here we introduce a facile method that successfully prevents this aging behaviour and enables accessing the systems' liquid-crystal and crystalline phases. We graft the comb-like polymer, poly(L-lysine)-g-poly(ethylene glycol) (PLL-PEG), onto the clay surfaces from solution, thereby screening the negative surface charges and thus ensuring steric stabilisation. We show zeta-sizer and rheology measurements, respectively, confirming complete steric coating and that aging of dilute samples is completely suppressed even after a year. Using evaporation as means to concentrate the particles, we observe various liquid crystalline textures under a polarized optical microscope (POM). Upon sequential spreading and drying, we are also able to obtain transparent films with hierarchical architecture.

cond-mat.soft↗
arXiv2017

Colloidal Motion under the Action of a Thermophoretic Force

We present thermophoretic measurements in aqueous suspensions of three different polystyrene (PS) particles of varying negative charge, size and surface coating. Our measurement technique is based on the observation of the colloidal steady-state distribution using conventional bright-field microscopy, which avoids undesirable effects such as laser-induced convection or local heating. We find that the colloids with the weakest zeta potential exhibit the strongest thermophoretic effect, suggesting that surface functionality leads to a more intricate dependence of the Soret coefficient on hydrodynamic boundary conditions than predicted by existing theoretical approaches. We also study the relaxation of the colloids to steady-state and propose a model to quantify the relaxation speed, based on the time evolution of the colloidal center of mass. Our observations are well described by this model and show that the relaxation speed tends to increase with the magnitude of the thermophoretic force.

cond-mat.soft↗
arXiv2017

Optical trapping of colloids at a liquid-liquid interface

We demonstrate the realization of (laterally) optically bounded colloidal structures on a liquid-liquid interface of an emulsion droplet. We use DNA tethers to graft the particles to the droplet surface, effectively confining them to a quasi-2D plane with minimum constraints on the lateral movement even when optically trapped in a common single-beam configuration. We show that relatively weak interactions such as depletion can be measured in the optically bounded crystals by video-microscopy imaging and analysis. This illustrates the possible use of our system as template to study optically controlled quasi two-dimensional colloidal assembly on liquid-liquid interfaces.

cond-mat.soft↗
arXiv2016

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

We report a study of reversible adsorption of DNA-coated colloids on complementary functionalized oil droplets. We show that it is possible to control the surface coverage of oil droplets by colloidal particles, by exploiting the fact that during slow adsorption, compositional arrest takes place well before structural arrest occurs. As a consequence, we can prepare colloid-coated oil droplets with a `frozen' degree of loading, but with fully ergodic colloidal dynamics on the droplets. We illustrate the equilibrium nature of the adsorbed colloidal phase by exploring the quasi two-dimensional (2d) phase behaviour of the adsorbed colloids under the influence of depletion interactions. We present simulations of a simple model that illustrates the nature of the compositional arrest and the structural ergodicity.

cond-mat.soft↗
arXiv2015

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

Short DNA linkers are increasingly being exploited for driving specific self-assembly of Brownian objects. DNA-functionalised colloids can assemble into ordered or amorphous materials with tailored morphology. Recently, the same approach has been applied to compliant units, including emulsion droplets and lipid vesicles. The liquid structure of these substrates introduces new degrees of freedom: the tethers can diffuse and rearrange, radically changing the physics of the interactions. Unlike droplets, vesicles are extremely deformable and DNA-mediated adhesion causes significant shape adjustments. We investigate experimentally the thermal response of pairs and networks of DNA-tethered liposomes and observe two intriguing and possibly useful collective properties: negative thermal expansion and tuneable porosity of the liposome networks. A model providing a thorough understanding of this unexpected phenomenon is developed, explaining the emergent properties out of the interplay between the temperature-dependent deformability of the vesicles and the DNA-mediated adhesive forces.

cond-mat.soft↗
arXiv2013

Multistep kinetic self-assembly of DNA-coated colloids

Self-assembly is traditionally described as the process through which an initially disordered system relaxes towards an equilibrium ordered phase only driven by local interactions between its building blocks. However, This definition is too restrictive. Nature itself provides examples of amorphous, yet functional, materials assembled upon kinetically arresting the pathway towards the ground state. Kinetic self-assembly is intrinsically more flexible and reliable than its equilibrium counterpart, allowing control over the morphology of the final phase by tuning both the interactions and the thermodynamic pathway leading to kinetic arrest. Here we propose strategies to direct the gelation of two-component colloidal mixtures by sequentially activating selective interspecies and intra-species interactions. We investigate morphological changes in the structure of the arrested phases by means of event driven molecular dynamics (MD) simulations and experimentally using DNA-coated colloids (DNACCs). Our approach can be exploited to finely tune the morphology of multicomponent nano- or micro-porous materials with possible applications in hybrid photovoltaics, photonics and drug delivery.

cond-mat.soft↗
arXiv2012

Layering, freezing and re-entrant melting of hard spheres in soft confinement

Confinement can have a dramatic effect on the behavior of all sorts of particulate systems and it therefore is an important phenomenon in many different areas of physics and technology. Here, we investigate the role played by the softness of the confining potential. Using grand canonical Monte Carlo simulations, we determine the phase diagram of three-dimensional hard spheres that in one dimension are constrained to a plane by a harmonic potential. The phase behavior depends strongly on the density and on the stiffness of the harmonic confinement. Whilst we find the familiar sequence of confined hexagonal and square-symmetric packings, we do not observe any of the usual intervening ordered phases. Instead, the system phase separates under strong confinement, or forms a layered re-entrant liquid phase under weaker confinement. It is plausible that this behavior is due to the larger positional freedom in a soft confining potential and to the contribution that the confinement energy makes to the total free energy. The fact that specific structures can be induced or suppressed by simply changing the confinement conditions (e.g. in a dielectrophoretic trap) is important for applications that involve self-assembled structures of colloidal particles.

cond-mat.soft↗
arXiv2011

Interactions between colloids induced by a soft cross-linked polymer substrate

Using video-microscopy imaging we demonstrate the existence of a short-ranged equilibrium attraction between heavy silica colloids diffusing on soft surfaces of cross-linked polymer gels. The inter-colloid potential can be tuned by changing the gel stiffness or by coating the colloids with a polymer layer. On sufficiently soft substrates, the interaction induced by the polymer matrix leads to large-scale colloidal aggregation. We correlate the in-plane interaction with a colloid-surface attraction.

cond-mat.soft↗
arXiv2010

Real-time monitoring of complex moduli from micro-rheology

We describe an approach to online analysis of micro-rheology data using a multi-scale time-correlation method. The method is particularly suited to process high-volume data streams and compress the relevant information in real time. Using this, we can obtain complex moduli of visco-elastic media without suffering from the high-frequency artefacts that are associated with the truncation errors in the most widely used versions of micro-rheology. Moreover, the present approach obviates the need to choose the time interval for data acquisition beforehand. We test our approach first on an artificial data set and then on experimental data obtained both for an optically trapped colloidal probe in water and a similar probe in poly-ethylene glycol solutions at various concentrations. In all cases, we obtain good agreement with the bulk rheology data in the region of overlap. We compare our method with the conventional Kramers-Kronig transform approach and find that the two methods agree over most of the frequency regime. For the same data set, the present approach is superior to Kramers-Kronig at high frequencies and can be made to perform at least comparable at low frequencies.

cond-mat.soft↗
arXiv2009

Colloidal Flying Carpets

DNA plays a special role in polymer science not just because of the highly selective recognition of complementary single DNA strands but also because bacteria can express DNA chains that are very long yet perfectly monodisperse. The latter reason makes long DNA molecules widely used as model systems in polymer science. Here, we report the unusual self-assembly that takes place in systems of colloids coated with very long double-stranded DNA. In particular, we find that colloids coated with such long DNA can assemble into unique floating crystalline monolayers. Floating colloidal structures have potentially interesting applications as such ordered structures can be assembled in one location and then deposited somewhere else. This would open the way to the assembly of multi-component, layered colloidal crystals.

cond-mat.soft↗
arXiv2006

Fluctuation-dissipation theorem in an aging colloidal glass

We provide a direct experimental test of the Stokes-Einstein relation as a special case of the fluctuation-dissipation theorem (FDT) in an aging colloidal glass. The use of combined active and passive microrheology allows us to independently measure both the correlation and response functions in this non-equilibrium situation. Contrary to previous reports, we find no deviations from the FDT over several decades in frequency (1 Hz-10 kHz) and for all aging times. In addition, we find two distinct viscoelastic contributions in the aging glass, including a nearly elastic response at low frequencies that grows during aging. This is the clearest change in material properties of the system with aging.

cond-mat.soft↗