arXiv subjects

Peter Schall

Publications and source records attributed to Peter Schall.

At least 37 records · Page 2Linked to original sources

arXiv2020

Nonequilibrium continuous phase transition in colloidal gelation with short-range attraction

The dynamical arrest of attractive colloidal particles into out-of-equilibrium structures, known as gelation, is central to biophysics, materials science, nanotechnology, and food and cosmetic applications, but a complete understanding is lacking. In particular, for intermediate particle density and attraction, the structure formation process remains unclear. Here, we show that the gelation of short-range attractive particles is governed by a nonequilibrium percolation process. We combine experiments on critical Casimir colloidal suspensions, numerical simulations, and analytical modeling with a master kinetic equation to show that cluster sizes and correlation lengths diverge with exponents 1.6 and 0.8, respectively, consistent with percolation theory, while detailed balance in the particle attachment and detachment processes is broken. Cluster masses exhibit power-law distributions with exponents -3/2 and -5/2 before and after percolation, as predicted by solutions to the master kinetic equation. These results revealing a nonequilibrium continuous phase transition unify the structural arrest and yielding into related frameworks.

cond-mat.soft↗

arXiv2019

Interevent time distributions of avalanche dynamics

Physical systems characterized by stick-slip dynamics often display avalanches. Regardless of the diversity of their microscopic structure, these systems are governed by a power-law distribution of avalanche size and duration. Here we focus on the interevent times between avalanches and show that, unlike their distributions of size and duration, the interevent time distributions are able to distinguish different mechanical states of the system, characterized by different volume fractions or confining pressures. We use experiments on granular systems and numerical simulations of emulsions to show that systems having the same probability distribution for avalanche size and duration can have different interevent time distributions. Remarkably, for large packing ratios, these interevent time distributions look similar to those for earthquakes and are indirect evidence of large space-time correlations in the system. Our results therefore indicate that interevent time statistics are more informative to characterize the dynamics of avalanches.

cond-mat.soft↗

arXiv2019

Buckling of self-assembled colloidal structures

Although buckling is a prime route to achieve functionalization and synthesis of single colloids, buckling of colloidal structures---made up of multiple colloids---remains poorly studied. Here, we investigate the buckling of the simplest form of a colloidal structure, a colloidal chain that is self-assembled through critical Casimir forces. We demonstrate that the mechanical instability of such a chain is strikingly reminiscent of that of classical Euler buckling but with thermal fluctuations and plastic effects playing a significant role. Namely, we find that fluctuations tend to diverge close to the onset of buckling and that plasticity controls the buckling dynamics at large deformations. Our work provides insight into the effect of geometrical, thermal and plastic interactions on the nonlinear mechanics of self-assembled structures, of relevance for the rheology of complex and living matter and the rational design of colloidal architectures.

cond-mat.soft↗

arXiv2018

On a critical artifact in the quantum yield methodology

For the development and optimization of novel light emitting materials, such as fluorescent proteins, dyes and semiconductor quantum dots (QDs), a reliable and robust analysis of the emission efficiency is crucial. The emission efficiency is typically quantified by the photoluminescence quantum yield (QY), defined by the ratio of emitted to absorbed photons. We show that this methodology suffers from a flaw that leads to underestimated QY values, presenting as a 'parasitic absorption'. This effect has not been described and/or corrected for in literature and is present already under common experimental conditions, therefore, it is highly relevant for a number of published studies. To correct for this effect, we propose a modification to the methodology and a correction procedure.

physics.app-ph↗

arXiv2018

Long-range strain correlations in 3D quiescent glass forming liquids

We present a quantitative study of strain correlations in quiescent supercooled liquids and glasses. Recent two-dimensional computer simulations and experiments indicate that even supercooled liquids exhibit long-lived, long-range strain correlations. Here we investigate this issue in three dimensions via experiments on hard sphere colloids and molecular dynamics simulations of a glass forming binary Lennard Jones mixture. Both in the glassy state and in the supercooled regime, strain correlations are found to decay with a $1/r^{3}$ power-law behavior, reminiscent of elastic fields around an inclusion. Moreover, theoretical predictions on the time dependence of the correlation amplitude are in line with the results obtained from experiments and simulations. It is argued that the size of the domain, which exhibits a "solid-like" cooperative strain pattern in a supercooled liquid, is determined by the product of the speed of sound with the structural relaxation time. While this length is of the order of nanometers in the normal liquid state, it grows to macroscale when approaching the glass transition.

cond-mat.stat-mech↗

arXiv2017

Direct Observation of Entropic Stabilization of bcc Crystals Near Melting

Crystals with low latent heat are predicted to melt from an entropically stabilized body-centered cubic symmetry. At this weakly first-order transition, strongly correlated fluctuations are expected to emerge, which could change the nature of the transition. Here we show how large fluctuations stabilize bcc crystals formed from charged colloids, giving rise to strongly power-law correlated heterogeneous dynamics. Moreover, we find that significant nonaffine particle displacements lead to a vanishing of the nonaffine shear modulus at the transition. We interpret these observations by reformulating the Born-Huang theory to account for nonaffinity, illustrating a scenario of ordered solids reaching a state where classical lattice dynamics fail.

cond-mat.soft↗

arXiv2017

Direct observation of percolation in the yielding transition of colloidal glasses

When strained beyond the linear regime, soft colloidal glasses yield to steady-state plastic flow in a way that is similar to the deformation of conventional amorphous solids. Due to the much larger size of the colloidal particles with respect to the atoms comprising an amorphous solid, colloidal glasses allow to obtain microscopic insight into the nature of the yielding transition, as we illustrate here combining experiments, atomistic simulations, and mesoscopic modeling. Our results unanimously show growing clusters of non-affine deformation percolating at yielding. In agreement with percolation theory, the spanning cluster is fractal with a fractal dimension d_f~2, and the correlation length diverges upon approaching the critical yield strain. These results indicate that percolation of highly non-affine particles is the hallmark of the yielding transition in disordered glassy systems.

cond-mat.soft↗

arXiv2016

Measuring nonlinear stresses generated by defects in 3D colloidal crystals

The mechanical, structural and functional properties of crystals are determined by their defects and the distribution of stresses surrounding these defects has broad implications for the understanding of transport phenomena. When the defect density rises to levels routinely found in real-world materials, transport is governed by local stresses that are predominantly nonlinear. Such stress fields however, cannot be measured using conventional bulk and local measurement techniques. Here, we report direct and spatially resolved experimental measurements of the nonlinear stresses surrounding colloidal crystalline defect cores, and show that the stresses at vacancy cores generate attractive interactions between them. We also directly visualize the softening of crystalline regions surrounding dislocation cores, and find that stress fluctuations in quiescent polycrystals are uniformly distributed rather than localized at grain boundaries, as is the case in strained atomic polycrystals. Nonlinear stress measurements have important implications for strain hardening, yield, and fatigue.

cond-mat.mtrl-sci↗

arXiv2014

The Boson Peak and Disorder in Hard Sphere Colloidal Systems

The Boson peak is believed to be the key to the fundamental understanding of the anomalous thermodynamic properties of glasses, notably the anomalous peak in the heat capacity at low temperatures; it is believed to be due to an excess of low frequency vibrational modes and a manifestation of the structural disorder in these systems. We study the thermodynamics and vibrational dynamics of colloidal glasses and (defected) crystals. The experimental determination of the vibrational density of states allows us to directly observe the Boson peak as a strong enhancement of low frequency modes. Using a novel method [Zargar et al., Phys. Rev. Lett. 110, 258301 (2013)] to determine the free energy, we also determine the entropy and the specific heat experimentally. It follows that the emergence of the Boson peak and high values of the specific heat are directly related and are specific to the glass: for a very defected crystal with a disorder that is only slightly smaller than for the glass, both the low-frequency density of states and the specific heat are significantly smaller than in the glass.

cond-mat.soft↗

arXiv2014

A criterion for condensation in kinetically constrained one-dimensional transport models

We study condensation in one-dimensional transport models with a kinetic constraint. The kinetic constraint results in clustering of immobile vehicles; these clusters can grow to macroscopic condensates, indicating the onset of dynamic phase separation between free flowing and arrested traffic. We investigate analytically the conditions under which this occurs, and derive a necessary and sufficient criterion for phase separation. This criterion is applied to the well-known Nagel-Schreckenberg model of traffic flow to analytically investigate the existence of dynamic condensates. We find that true condensates occur only when acceleration out of jammed traffic happens in a single time step, in the limit of strong overbraking. Our predictions are further verified with simulation results on the growth of arrested clusters. These results provide analytic understanding of dynamic arrest and dynamic phase separation in one-dimensional traffic and transport models.

cond-mat.stat-mech↗

arXiv2014

Correlations of plasticity in sheared glasses

In a recent paper [S. Mandal et al., Phys. Rev. E 88, 022129 (2013)] the nature of spatial correlations of plasticity in hard sphere glasses was addressed both via computer simulations and in experiments. It was found that the experimentally obtained correlations obey a power law whereas the correlations from simulations are better fitted by an exponential decay. We here provide direct evidence--- via simulations of a hard sphere glass in 2D---that this discrepancy is a consequence of the finite system size in the 3D simulations. By extending the study to a 2D soft disk model at zero temperature, the robustness of the power-law decay in sheared amorphous solids is underlined. Deviations from a power law occur when either reducing the packing fraction towards the supercooled regime in the case of hard spheres or changing the dissipation mechanism from contact dissipation to a mean-field type drag for the case of soft disks.

cond-mat.soft↗

arXiv2013

Visualizing the strain evolution during the indentation of colloidal glasses

We use an analogue of nanoindentation on a colloidal glass to elucidate the incipient plastic deformation of glasses. By tracking the motion of the individual particles in three dimensions, we visualize the strain field and glass structure during the emerging deformation. At the onset of flow, we observe a power-law distribution of strain indicating strongly correlated deformation, and reflecting a critical state of the glass. At later stages, the strain acquires a Gaussian distribution, indicating that plastic events become uncorrelated. Investigation of the glass structure using both static and dynamic measures shows a weak correlation between the structure and the emerging strain distribution. These results indicate that the onset of plasticity is governed by strong power-law correlations of strain, weakly biased by the heterogeneous glass structure.

cond-mat.soft↗

arXiv2013

Single particle fluctuations and directional correlations in driven hard sphere glasses

Via event driven molecular dynamics simulations and experiments, we study the packing fraction and shear-rate dependence of single particle fluctuations and dynamic correlations in hard sphere glasses under shear. At packing fractions above the glass transition, correlations increase as shear rate decreases: the exponential tail in the distribution of single particle jumps broadens and dynamic four-point correlations increase. Interestingly, however, upon decreasing the packing fraction, a broadening of the exponential tail is also observed, while dynamic heterogeneity is shown to decrease. An explanation for this behavior is proposed in terms of a competition between shear and thermal fluctuations. Building upon our previous studies [Chikkadi et al, Europhys. Lett. (2012)], we further address the issue of anisotropy of the dynamic correlations.

cond-mat.soft↗

arXiv2013

Dynamics of colloidal aggregation in microgravity by critical Casimir forces

Using the critical Casimir force, we study the attractive-strength dependence of diffusion-limited colloidal aggregation in microgravity. By means of near field scattering we measure both the static and dynamic structure factor of the aggregates as the aggregation process evolves. The simultaneous measurement of both the static and dynamic structure factor under ideal microgravity conditions allows us to uniquely determine the ratio of the hydrodynamic and gyration radius as a function of the fractal dimension of the aggregate, enabling us to elucidate the internal structure of the aggregates as a function of the interaction potential. We find that the mass is evenly distributed in all objects with fractal dimension ranging from 2.55 for a shallow to 1.75 for the deepest potential.

cond-mat.soft↗

arXiv2013

Direct Measurement of the Free Energy of Aging Hard-Sphere Colloidal Glasses

The nature of the glass transition is one of the most important unsolved problems in condensed matter physics. The difference between glasses and liquids is believed to be caused by very large free energy barriers for particle rearrangements; however so far it has not been possible to confirm this experimentally. We provide the first quantitative determination of the free energy for an aging hard-sphere colloidal glass. The determination of the free energy allows for a number of new insights in the glass transition, notably the quantification of the strong spatial and temporal heterogeneity in the free energy. A study of the local minima of the free energy reveals that the observed variations are directly related to the rearrangements of the particles. Our main finding is that the probability of particle rearrangements shows a power law dependence on the free energy changes associated with the rearrangements, similarly to the Gutenberg-Richter law in seismology.

cond-mat.soft↗

arXiv2013

Controlling colloidal phase transitions with critical Casimir forces

The critical Casimir effect provides a thermodynamic analogue of the well-known quantum mechanical Casimir effect. It acts between two surfaces immersed in a critical binary liquid mixture, and results from the confinement of concentration fluctuations of the solvent. Unlike the quantum mechanical effect, the magnitude and range of this attraction can be adjusted with temperature via the solvent correlation length, thus offering new opportunities for the assembly of nano and micron-scale structures. Here, we demonstrate the active assembly control of equilibrium phases using critical Casimir forces. We guide colloidal particles into analogues of molecular liquid and solid phases via exquisite control over their interactions. By measuring the critical Casimir particle pair potential directly from density fluctuations in the colloidal gas, we obtain insight into liquefaction at small scales: We apply the Van der Waals model of molecular liquefaction and show that the colloidal gas-liquid condensation is accurately described by the Van der Waals theory, even on the scale of a few particles. These results open up new possibilities in the active assembly control of micro and nanostructures.

cond-mat.soft↗

arXiv2012

Colloidal aggregation in microgravity by critical Casimir forces

By using the critical Casimir force, we study the attractive strength dependent aggregation of colloids with and without gravity by means of Near Field scattering. Significant differences were seen between microgravity and ground experiments, both in the structure of the formed fractal aggregates as well as the kinetics of growth. Ground measurements are severely affected by sedimentation resulting in reaction limited behavior. In microgravity, a purely diffusive behavior is seen reflected both in the measured fractal dimensions for the aggregates as well as the power law behavior in the rate of growth. Formed aggregates become more open as the attractive strength increases.

cond-mat.soft↗

arXiv2011

Long-range strain correlations in sheared colloidal glasses

Glasses behave as solids on experimental time scales due to their slow relaxation. Growing dynamic length scales due to cooperative motion of particles are believed to be central to this slow response. For quiescent glasses, however, the size of the cooperatively rearranging regions has never been observed to exceed a few particle diameters, and the observation of long-range correlations that are signatures of an elastic solid has remained elusive. Here, we provide direct experimental evidence of long-range correlations during the deformation of a dense colloidal glass. By imposing an external stress, we force structural rearrangements that make the glass flow, and we identify long-range correlations in the fluctuations of microscopic strain, and elucidate their scaling and spatial symmetry. The applied shear induces a transition from homogeneous to inhomogeneous flow at a critical shear rate, and we investigate the role of strain correlations in this transition.

cond-mat.soft↗