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Peter Schurtenberger

Publications and source records attributed to Peter Schurtenberger.

27 records · Page 2Linked to original sources

Unexpected decoupling of stretching and bending modes in protein gels

We show that gels formed by arrested spinodal decomposition of protein solutions exhibit elastic properties in two distinct frequency domains, both elastic moduli exhibiting a remarkably strong dependence on volume fraction. Considering the large difference between the protein size and the characteristic length of the network we model the gels as porous media and show that the high and low frequency elastic moduli can be respectively attributed to stretching and bending modes. The unexpected decoupling of the two modes in the frequency domain is attributed to the length scale involved: while stretching mainly relates to the relative displacement of two particles, bending involves the deformation of a strand with a thickness of the order of a thousand particle diameters.

cond-mat.soft↗

Phase separation and dynamical arrest for particles interacting with mixed potentials--the case of globular proteins revisited

We examine the applicability of the extended law of corresponding states (ELCS) to equilibrium and non equilibrium features of the state diagram of the globular protein lysozyme. We provide compelling evidence that the ELCS correctly reproduces the location of the binodal for different ionic strengths, but fails in describing the location of the arrest line. We subsequently use Mode Coupling Theory (MCT) to gain additional insight into the origin of these observations. We demonstrate that while the critical point and the connected binodal and spinodal are governed by the integral features of the interaction potential described by the normalized second virial coefficient, the arrest line is mainly determined by the attractive well depth or bond strength. This article is published in Soft Matter. The reference is: DOI: 10.1039/c0sm01175d

cond-mat.soft↗

A closer look at arrested spinodal decomposition in protein solutions

Concentrated aqueous solutions of the protein lysozyme undergo a liquid solid transition upon a temperature quench into the unstable spinodal region below a characteristic arrest temperature of Tf=15C. We use video microscopy and ultra-small angle light scattering in order to investigate the arrested structures as a function of initial concentration, quench temperature and rate of the temperature quench. We find that the solid-like samples show all the features of a bicontinuous network that is formed through an arrested spinodal decomposition process. We determine the correlation length Xi and demonstrate that Xi exhibits a temperature dependence that closely follows the critical scaling expected for density fluctuations during the early stages of spinodal decomposition. These findings are in agreement with an arrest scenario based on a state diagram where the arrest or gel line extends far into the unstable region below the spinodal line. Arrest then occurs when during the early stage of spinodal decomposition the volume fraction phi2 of the dense phase intersects the dynamical arrest threshold phi2Glass, upon which phase separation gets pinned into a space-spanning gel network with a characteristic length Xi.

cond-mat.soft↗

Interplay between Spinodal Decomposition and Glass Formation in Proteins Exhibiting Short-Range Attractions

We investigate the competition between spinodal decomposition and dynamical arrest using aqueous solutions of the globular protein lysozyme as a model system for colloids with short-range attractions. We show that quenches below a temperature Ta lead to gel formation as a result of a local arrest of the proteindense phase during spinodal decomposition. The rheological properties of these gels allow us to use centrifugation experiments to determine the local densities of both phases and to precisely locate the gel boundary and the attractive glass line close to and within the unstable region of the phase diagram.

cond-mat.soft↗

A simple patchy colloid model for the phase behavior of lysozyme dispersions

We propose a minimal model for spherical proteins with aeolotopic pair interactions to describe the equilibrium phase behavior of lysozyme. The repulsive screened Coulomb interactions between the particles are taken into account assuming that the net charges are smeared out homogeneously over the spherical protein surfaces. We incorporate attractive surface patches, with the interactions between patches on different spheres modeled by an attractive Yukawa potential. The parameters entering the attractive Yukawa potential part are determined using information on the experimentally accessed gas-liquid-like critical point. The Helmholtz free energy of the fluid and solid phases is calculated using second-order thermodynamic perturbation theory. Our predictions for the solubility curve are in fair agreement with experimental data. In addition, we present new experimental data for the gas-liquid coexistence curves at various salt concentrations and compare these with our model calculations. In agreement with earlier findings, we observe that the strength and the range of the attractive potential part only weakly depend on the salt content.

cond-mat.soft↗

Engineering solid-like structures via an arrested spinodal decomposition

The possibilities to tune the structure of solid like material resulting from arrested spinodal decomposition is investigated using a system composed of lysozyme, a globular protein, dispersed in a water solution as model system for colloids with short range attraction. It is shown that the resulting arrested spinodal decomposition is driven by the interplay between the early kinetics of the spinodal decomposition and the dynamical arrest. The initial concentration, the quench depth and speed from the fluid state to the arrested state enable to tailor the mesh size of the solid network of the arrested spinodal decomposition.

cond-mat.soft↗

Density-dependent interactions and structure of charged colloidal dispersions in the weak screening regime

We determine the structure of charge-stabilized colloidal suspensions at low ionic strength over an extended range of particle volume fractions using a combination of light and small angle neutron scattering experiments. The variation of the structure factor with concentration is analyzed within a one-component model of a colloidal suspension. We show that the observed structural behavior corresponds to a non-monotonic density dependence of the colloid effective charge and the mean interparticle interaction energy. Our findings are corroborated by similar observations from primitive model computer simulations of salt-free colloidal suspensions.

cond-mat.soft↗

Modeling Equilibrium Clusters in Lysozyme Solutions

We present a combined experimental and numerical study of the equilibrium cluster formation in globular protein solutions under no-added salt conditions. We show that a cluster phase emerges as a result of a competition between a long-range screened Coulomb repulsion and a short-range attraction. A simple effective potential, in which only depth and width of the attractive part of the potential are optimized, accounts in a remarkable way for the wavevector dependence of the X-ray scattering structure factor.

cond-mat.soft↗

Multiple scattering suppression in dynamic light scattering based on a digital camera detection scheme

We introduce a charge coupled device (CCD) camera based detection scheme in dynamic light scattering that provides information on the single-scattered auto-correlation function even for fairly turbid samples. It is based on the single focused laser beam geometry combined with the selective cross correlation analysis of the scattered light intensity. Using a CCD camera as a multispeckle detector we show how spatial correlations in the intensity pattern can be linked to single and multiple scattering processes. Multiple scattering suppression is then achieved by an efficient cross correlation algorithm working in real time with a temporal resolution down to 0.2 seconds. Our approach allows access to the extensive range of systems that show low-order scattering by selective detection of the singly scattered light. Model experiments on slowly relaxing suspensions of titanium dioxide in glycerol were carried out to establish the validity range of our approach. Successful application of the method is demonstrated up to a scattering coefficient of more than $μ_s = 5$ cm$^{-1}$ for the sample size of L=1 cm.

cond-mat.soft↗