arXiv subjects

Erika Eiser

Publications and source records attributed to Erika Eiser.

At least 19 recordsLinked to original sources

arXiv2026

DWS-based microrheology of triblock copolymers

The thermally reversible phase transitions in aqueous solutions of the triblock copolymers known as Pluronic and their related textures are well-researched. However, their corresponding rheological properties are less studied. In particular, their high-temperature behavior is difficult to access with classical rheology. Here we demonstrated that Diffusing Wave Spectroscopy (DWS)-based microrheology allows us to study the phase transition and the associated viscoelastic properties of Pluronic F127 solutions for temperatures from 5 C to 80 C. From the measured intensity-autocorrelation functions we can extract effective viscosities and determine the critical micellization temperature and concentration. Moreover,the high EO/PO (arm-to-core) ratio of F127 and its polydispersity play a critical role in the high-temperature re-entrant liquid phase, due to decreasing solubility of PEO along with the dehydration of the PPO core. The microscopic viscoelastic moduli G'({\omega}) and G''({\omega}) help to determine these phase transitions and provide mechanical properties in the solid phase that are not readily accessible with standard multi-particle tracking techniques due to limited Brownian motion.

cond-mat.soft↗

arXiv2026

Arc-length characterization of finite, radial growth patterns

We present a method to characterize the distribution of length-scales of finite, disordered patterns with, on average, radial symmetry. This method makes it possible to quantify the distribution of characteristic length scales in cases where the conventional "linear" chord method does not work. We show that the method can clearly distinguish regular patterns, patterns that are formed by diffusion-limited aggregation, and patterns that form during the slow drying of confined, colloid-laden droplets, explained by Beechey-Newman et al.1 We also introduce a method to find the centre-point of these finite patterns, without assuming a full connectivity in the pattern. The method should be widely applicable to other, finite quasi-two-dimensional patterns like dendritic structures, viscous fingering, liquid crystal patterns and bacterial growth.

cond-mat.soft↗

arXiv2025

Heat and super-diffusive melting fronts in unsaturated porous media

When water is present in a medium with pore sizes in a range around 10nm the corresponding freezing point depression will cause long range broadening of a melting front. Describing the freezing-point depression by the Gibbs-Thomson equation and the pore size distribution by a power law, we derive a non-linear diffusion equation for the fraction of melted water. This equation yields super-diffusive spreading of the melting front with a diffusion exponent which is given by the spatial dimension and the exponent describing the pore size distribution. We derive this solution analytically from energy conservation in the limit where all the energy is consumed by the melting and explore the validity of this approximation numerically. Finally, we explore a geological application of the theory to the case of one-dimensional sub-surface melting fronts in granular or soil systems. These fronts, which are produced by heating of the surface, spread at a super-diffusive rate and affect the subsurface to significantly larger depths than would a system without the effects of freezing point depression.

cond-mat.soft↗

arXiv2025

Confined colloidal droplets dry to form circular mazes

During drying, particle-laden sessile droplets will leave so-called coffee-stain rings behind. This phenomenon is well-known and well-understood (Deegan et al., Nature 389, 827-829 (1997)). Here we show that when particle-laden droplets confined in a slit are allowed to evaporate very slowly, they do not deposit coffee rings, but form a surprisingly intricate, circular maze-like pattern. We present experiments that illustrate this pattern formation and discuss the factors that determine when such patterns can form. We are not aware of reports of natural examples of the formation of such beautiful patterns under confinement, although it seems likely that they exist.

cond-mat.soft↗

arXiv2023

Towards New Liquid Crystal Phases of DNA mesogens

Short, partially complementary, single-stranded (ss)DNA strands can form nanostructures with a wide variety of shapes and mechanical properties. It is well known that semiflexible, linear dsDNA can undergo an isotropic to nematic (IN) phase transition and that sufficiently bent structures can form a biaxial nematic phase. Here we use numerical simulations to explore how the phase behaviour of linear DNA constructs changes as we tune the mechanical properties of the constituent DNA by changing the nucleotide sequence. The IN phase transition can be suppressed in so-called DNA 'nunchakus': structures consisting of two rigid dsDNA arms, separated by a sufficiently flexible spacer. In this paper, we use simulations to explore what phase behavior to expect for different linear DNA constructs. To this end, we first performed numerical simulations exploring the structural properties of a number of different DNA oligonucleotides, using the oxDNA package. We then used the structural information generated in the oxDNA simulations to construct more coarse-grained models of the rodlike, bent-core, and nunchaku DNA. These coarse-grained models were used to explore the phase behavior of suspensions of the various DNA constructs. The approach explored in this paper makes it possible to 'design' the phase behavior of DNA constructs by a suitable choice of the constituent nucleotide sequence.

cond-mat.soft↗

arXiv2022

Dynamic Light Scattering based microrheology of End-functionalised triblock copolymer solutions

'Soft' patchy surfactant micelles have become an additional building tool in self-assembling systems. The triblock copolymer, Pluronic F108, forms spherical micelles in aqueous solutions upon heating leading to a simple phase diagram with a micellar crystalline solid at higher temperatures and concentrations. Here we report the strong influence of end-functionalising the chain ends either with an azide or azide-DNA complex on the systems' phase behaviour. We find that the azide(N3)- functionalisation renders the chain ends weakly hydrophobic at lower temperatures, causing them to self-assemble into flower-micelles. This hydrophobicity increases with increasing temperature and poses a competing self-assembling mechanism to the solvent induces hydrophobic interactions between the middle-blocks of F108 at higher temperatures and leads to a macroscopic phase separation that is absent in the pure F108 system. However, when we attached short, hydrophilic single-stranded (ss)DNA to the azide groups via click chemistry the chain ends became 'sticky' due to DNA hybridisation below the melting temperature of the complementary ssDNA ends while reverting to hydrophilic behaviour above. We characterise their structural and rheological properties via Dynamic Light Scattering (DLS) and DLS-based passive microrheology with an improved time-frequency domain inversion step. We present the structural behaviour of dilute and semi-dilute solutions of the original F108 system and compare the results with solutions containing either the F108- azide (F108-N3) or partially DNA-functionalised F108-azide chains. Our DLS and microrheology studies inform us on how the attachment of azide groups on F108 changes the mechanical and structural properties of micellar fluids pioneering further characterisation and design of these hybrid systems.

cond-mat.soft↗

arXiv2022

Kinetically limited valence of colloidal particles with surface mobile DNA linkers

We characterize the self-assembly of colloidal particles with surface mobile DNA linkers under kinetically limited valence conditions. For this, we put forward a computer simulation model that captures quantitatively the interplay between the main dynamic processes governing these systems and allows the simulation of the long time scales reached in experiments. The model is validated by direct comparison with available experimental results, showing an overall good agreement that includes measurements of the average effective valence and its probability distribution as a function of the density of DNA linkers on the particles surface. Finally, simulation results are used to evidence the opposite impact of particle density and characteristic DNA hybridization time on the effective valence.

cond-mat.soft↗

arXiv2021

Elastic Response of Wire Frame Glasses. I. Two Dimensional Model

We study the elastic response of concentrated suspensions of rigid wire frame particles to a step strain. These particles are constructed from infinitely thin, rigid rods of length $L$. We specifically compare straight rod-like particles to bent and branched wire frames. In dense suspensions the wire frames are frozen in a disordered state by the topological entanglements between their arms. We present a simple, geometric method to find the scaling of the elastic stress with concentration in these glassy systems. We apply this method to a simple 2D model system where a test particle is placed on a plane and constrained by a random distribution of points with number density $ν$. Two striking differences between wire frame and rod suspensions are found: 1) The linear elasticity per particle for wire frames is very large, scaling like $ν^2 L^4$, whereas for rods it much smaller and independent of concentration. 2) Rods always shear thin but wire frames shear harden for densities less than $\sim \sqrt{K/k_B T L^4}$, where $K$ is the bending modulus of the particles. The deformation of wire frames is found to be important even for small strains, with the proportion of deformed particles at a particular strain, $γ$, being given by $(νL^2)^2 γ^2$. Our results agree well with a simple simulation of the 2D system.

cond-mat.soft↗

arXiv2021

Elastic Response of Wire Frame Glasses. II. Three Dimensional Systems

We study the elastic response of rigid, wire frame particles in concentrated, glassy suspensions to a step strain by applying the simple, geometric methods developed in part I. The wire frame particles are comprised of thin, rigid rods of length $L$ and their number density, $ρ$, is such that $ρL^3 \gg 1$. We specifically compare rigid rods to L-shapes made of two equal length rods joined at right angles. The behaviour of wire frames is found to be strikingly different from that of rods. The linear elasticity scales like $ρ^3 L^6$ for L-shaped particles, whereas it scales proportional to $ρ$ for rods and the non-linear response shows a transition from shear hardening to shear softening at a critical density $ρ_c \sim \sqrt{K / k_B T L^6}$, where $K$ is the bending modulus of the particles. For realistic particles made of double stranded DNA, this transition occurs at densities of about $ρL^3 \sim 10$. The reason for these differences is that wire frames can be forced to bend by the entanglements with their surroundings, whereas rods always remain straight. This is found to be very important even for small strains, with most particles being bent above a critical strain $γ_c \sim (ρL^3)^{-1}$.

cond-mat.soft↗

arXiv2020

Controlled Optofluidic Crystallization of Colloids Tethered at Interfaces

We report experiments that show rapid crystallization of colloids tethered to an oil-water interface in response to laser illumination. This light-induced transition is due to a combination of long-ranged thermophoretic pumping and local optical binding. We show that the flow-induced force on the colloids can be described as the gradient of a potential. The nonequilibrium steady state due to local heating thus admits an effective equilibrium description. The optofluidic manipulation explored in this work opens novel ways to manipulate and assemble colloidal particles

cond-mat.soft↗

arXiv2020

Inhibiting amyloid-like aggregation through bio-conjugation of proteins with polymer surfactant

Prevention of protein aggregation and thus stabilization of proteins has large biological and biotechnological implications. Here, we show that inhibition of amyloid-like aggregates is possible in stoichiometric conjugates of polymer surfactant and bovine serum albumin (BSA) chosen as a model protein. We investigate using a combination of Thioflavin-T fluorescence spectroscopy, dynamic light scattering and FTIR spectroscopy the aggregation behavior in polymer surfactant modified and unmodified (native) BSA solutions. The BSA-polymer surfactant conjugates are stable up to 5 days under aggregation conditions, while native BSA forms amyloid fibrillar structures. Further, DLS-based micro-rheology studies performed with heat-treated 100 to 200 μM native BSA aggregates provided understanding of the equilibrium elastic and viscous moduli over a very large frequency range, reaching MHz, which are inaccessible using bulk rheology. Our results indicate that after 6 days of aggregation conditions, elastic moduli showed values between 1.2 to 3.6 Pa corresponding to an entanglement length (ξ) of 105 nm. Interestingly, heating 200 μM native BSA solution at 65 degree C for 2 days in a plastic Eppendorf resulted in self-standing films. These films exhibited strong ThT-fluorescence intensity and a predominant \b{eta}-sheet secondary structure from the FTIR studies, suggesting that self-standing microstructure resulted from hierarchical self-assembly of amyloid fibrils.

q-bio.BM↗

arXiv2019

Particle shapes leading to Newtonian dilute suspensions

It is well known that suspensions of particles in a viscous fluid can affect the rheology significantly, producing a pronounced non-Newtonian response even in dilute suspension. However, it is unclear a priori which particle shapes lead to this behaviour. We present two simple symmetry conditions on the shape which are sufficient for a dilute suspension to be Newtonian for all strain sizes and one sufficient for Newtonian behavior for small strains. We also construct a class of shapes out of thin, rigid rods not found by the symmetry argument which share this property for small strains.

cond-mat.soft↗

arXiv2019

On the Role of Flexibility in Linker-Mediated DNA Hydrogels

Three-dimensional DNA networks, composed of tri- or higher valent nanostars with sticky, single-stranded DNA overhangs, have been previously studied in the context of designing thermally responsive, viscoelastic hydrogels. In this work, we use linker-mediated gels, where the sticky ends of two trivalent nanostars are connected through the complementary sticky ends of a linear DNA duplex. We can design this connection to be either rigid or flexible by introducing flexible, non-binding bases. The additional flexiblity provided by these non-binding bases influences the effective elasticity of the percolating gel formed at low temperatures. Here we show that by choosing the right length of the linear duplex and non-binding flexible joints, we obtain a completely different phase behaviour to that observed for rigid linkers. In particular, we use dynamic light scattering as microrheological tool to monitor the self-assembly of DNA nanostars with linear linkers as a function of temperature. While we observe classical gelation when using rigid linkers, the presence of flexible joints leads to a cluster fluid with reduced viscosity. Using both the oxDNA model and a coarse-grained simulation to investigate the nanostar-linker topology, we hypothesise on the possible structure formed by the DNA clusters.

physics.bio-ph↗

arXiv2019

A Numerical Study of Three-Armed DNA Hydrogel Structures

We present a numerical analysis of a DNA hydrogel that consists of three-valent Y-shaped DNA molecules. The building blocks self-assemble fully reversibly from complementary single-stranded DNA segments. We compare melting curves from both simulations with the oxDNA2 model and experiments and find excellent agreement. The morphology of the Y-DNA molecules is investigated when several alterations in the design are made. Adding inert nucleotides to the central core region of the Y-DNA molecules has a very minor effect on their overall geometry, whereas palindromic sequences in the sticky ends via which the individual Y-DNA molecules hybridize, have a profound influence on their relative twisting and bending angles.

cond-mat.soft↗

arXiv2018

Tunable colloidal photonic crystals

Spherical colloids arranged in a crystalline order are known to produce structural colors. The intensity and brilliance of such photonic crystals require high size-monodispersity of the colloids, a low number of lattice defects and disorder, as well as a relatively large refractive index contrast between the scattering colloids and the continuous background. Here we present the unexpected photonic properties of aqueous suspensions of charge-stabilized, 186 nm large, fluorinated colloids with a refractive index of 1.37. Employing reflectivity, optical observation, small angle x-ray scattering measurements and reflectivity modeling, we demonstrate that these suspensions become partially transparent while showing strong, almost angle-independent color in reflection despite the very small refractive index difference. Under certain conditions, additional sharp Bragg reflections are observed. We were able to tune the observed structural colors continuously across the entire visible range by simply changing the volume fraction of these colloidal suspensions, which show a white appearance when dilute, structural color and Bragg peaks when concentrated enough to form Wiegner crystal, and angle-independent color when very concentrated and in a glassy phase.

physics.optics↗

arXiv2018

A Facile Approach to Prepare Self-Assembled, Nacre-Inspired Clay/Polymer Nano-Composites

Nature provides many paradigms for the design and fabrication of artificial composite materials. Inspired by the relationship between the well-ordered architecture and biopolymers found in natural nacre, we present a facile strategy to construct large-scale organic/inorganic nacre-mimetics with hierarchical structure via a water-evaporation self-assembly process. Through hydrogen bonding, we connect Laponite-nanoclay platelets with each other using naturally abundant cellulose creating thin, flexible films with a local brick-and-mortar architecture. While the aqueous solution displays liquid crystalline textures, the dried films show a pronounced Young's modulus (9.09 GPa) with a maximum strength of 298.02 MPa and toughness of 16.63 MJm-3. In terms of functionalities, we report excellent glass-like transparency along with exceptional shape-persistent flame shielding. We also demonstrate that through metal ion-coordination we can further strengthen the interactions between the polymers and the nanoclays. These ion-treated hybrid films exhibit further enhanced mechanical, and thermal properties as well as resistance against swelling and dissolution in aqueous environments. We believe that our simple pathway to fabricate such versatile polymer/clay nanocomposites can open avenues for inexpensive production of environmentally friendly, biomimetic materials in aerospace, wearable electrical devices, artificial muscle, and food packaging industry.

cond-mat.soft↗

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↗