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Peter Keim

Publications and source records attributed to Peter Keim.

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Tracking shear mode dynamics across the glass transition in a 2D colloidal system

Long-wavelength collective shear dynamics are profoundly different in solids and liquids. According to the theoretical framework developed by Maxwell and Frenkel, collective shear waves vanish upon melting by acquiring a characteristic wave-vector gap, known as the $k$-gap. While this prediction has been supported by numerous simulations, experimental validation remains limited. Moreover, this phenomenon has been never tested across a continuous glass transition between a liquid phase and a glassy state with large but finite viscosity. In this work, we track the dispersion relation of collective shear modes in a two-dimensional colloidal system and provide direct experimental evidence for the emergence of a $k$-gap. This gap opens continuously at an effective temperature consistent with the onset of the glass transition and the vanishing of the static shear modulus. By extracting the instantaneous shear velocity from the experimental data, we uncover a shear relaxation time exhibiting a super-Arrhenius temperature dependence characteristic of glass-forming materials, accurately described by the Vogel-Fulcher-Tammann (VFT) relation. Our results confirm the predictions of the Maxwell-Frenkel framework and highlight their relevance across continuous melting processes originating from low-temperature amorphous solid phases.

cond-mat.soft

Symmetry breaking in two dimensions on ultra-fast time scales

Melting of two-dimensional mono-crystals is described within the celebrated Kosterlitz-Thouless-Halperin-Nelson-Young scenario (KTHNY-Theory) by the dissociation of topological defects. It describes the shielding of elasticity due to thermally activated topological defects until shear elasticity disappears. As a well defined continuous phase transition, freezing and melting should be reversible and independent of history. However, this is not the case: cooling an isotropic 2D fluid with a finite but nonzero rate does not end in mono-crystals. The symmetry can not be broken globally but only locally in the thermodynamic limit due to the critical slowing down of order parameter fluctuations. This results in finite sized domains with the same order parameter. For linear cooling rates, the domain size is described by the Kibble-Zurek mechanism, originally developed for the defect formation of the primordial Higgs-field shortly after the Big-Bang. In the present manuscript, we investigate the limit of the deepest descent quench on a colloidal monolayer and resolve the time dependence of structure formation for (local) symmetry breaking. Quenching to various target temperatures below the melting point (deep in the crystalline phase and just close to the transition), we find universal behaviour if the timescale is re-scaled properly.

cond-mat.soft

Tetratic Phase in 2D Crystals of Squares

Melting in 2D is described by the celebrated Kosterlitz-Thouless-Halperin-Nelson-Young (KTHNY) theory. The unbinding of two different types of topological defects destroys translational and orientational order at different temperatures. The intermediate phase is called hexatic and has been measured in 2D colloidal monolayers of isotropic particles. The hexatic is a fluid with six-fold quasi-long-ranged orientational order. Here, the melting of a quadratic, 4-fold crystal is investigated, consisting of squares of about $4 \times 4\;\mu\mathrm{m}$. The anisotropic particles are manufactured from a photoresist using a 3D nanoprinter. In aqueous solution, particles sediment by gravity to a thin cover slide where they form a monolayer. The curvature of the cover slide can be adjusted from convex to concave, which allows to vary the area density of the monolayer in the field of view. For low densities, the squares are free to diffuse and form a 2D fluid while for high densities they form a quadratic crystal. Using a four-fold bond-order correlation function, we resolve the tetratic phase with quasi long ranged orientational order.

cond-mat.soft

Experimental identification of topological defects in 2D colloidal glass

Topological defects are singularities within a field that cannot be removed by continuous transformations. The definition of these irregularities requires an ordered reference configuration, calling into question whether they exist in disordered materials, such as glasses. However, recent work suggests that well-defined topological defects emerge in the dynamics of glasses, even if they are not evident in the static configuration. In this study, we reveal the presence of topological defects in the vibrational eigenspace of a two-dimensional experimental colloidal glass. These defects strongly correlate with the vibrational features and spatially correlate with each other and structural "soft spots", more prone to plastic flow. This work experimentally confirms the existence of topological defects in disordered systems revealing the complex interplay between topology, disorder, and dynamics.

cond-mat.soft

Stealthy and hyperuniform isotropic photonic bandgap structure in 3D

In photonic crystals the propagation of light is governed by their photonic band structure, an ensemble of propagating states grouped into bands, separated by photonic band gaps. Due to discrete symmetries in spatially strictly periodic dielectric structures their photonic band structure is intrinsically anisotropic. However, for many applications, such as manufacturing artificial structural color materials or developing photonic computing devices, but also for the fundamental understanding of light-matter interactions, it is of major interest to seek materials with long range non-periodic dielectric structures which allow the formation of {\it isotropic} photonic band gaps. Here, we report the first ever 3D isotropic photonic band gap for an optimized disordered stealthy hyperuniform structure for microwaves. The transmission spectra are directly compared to a diamond pattern and an amorphous structure with similar node density. The band structure is measured experimentally for all three microwave structures, manufactured by 3D-Laser-printing for meta-materials with refractive index up to $n=2.1$. Results agree well with finite-difference-time-domain numerical investigations and a priori calculations of the band-gap for the hyperuniform structure: the diamond structure shows gaps but being anisotropic as expected, the stealthy hyperuniform pattern shows an isotropic gap of very similar magnitude, while the amorphous structure does not show a gap at all. The centimeter scaled microwave structures may serve as prototypes for micrometer scaled structures with bandgaps in the technologically very interesting region of infrared (IR).

physics.app-ph

Mermin-Wagner fluctuations in 2D amorphous solids

In a recent comment, M. Kosterlitz described how the discrepancy about the lack of broken translational symmetry in two dimensions - doubting the existence of 2D crystals - and the first computer simulations foretelling 2D crystals at least in tiny systems, motivated him and D. Thouless to investigate melting and suprafluidity in two dimensions [Jour. of Phys. Cond. Matt. \textbf{28}, 481001 (2016)]. The lack of broken symmetries proposed by D. Mermin and H. Wagner is caused by long wavelength density fluctuations. Those fluctuations do not only have structural impact but additionally a dynamical one: They cause the Lindemann criterion to fail in 2D and the mean squared displacement not to be limited. Comparing experimental data from 3D and 2D amorphous solids with 2D crystals we disentangle Mermin-Wagner fluctuations from glassy structural relaxations. Furthermore we can demonstrate with computer simulations the logarithmic increase of displacements predicted by Mermin and Wagner: periodicity is not a requirement for Mermin-Wagner fluctuations which conserve the homogeneity of space on long scales.

cond-mat.stat-mech

Strain pattern in supercooled liquids

Investigations of strain correlations at the glass transition reveal unexpected phenomena. The shear strain fluctuations show an Eshelby-strain pattern ($\,\sim \cos{(4θ)}/r^2\,$), characteristic for elastic response, even in liquids at long times [1]. We address this using a mode-coupling theory for the strain fluctuations in supercooled liquids and data from both, video microscopy of a two-dimensional colloidal glass former and simulations of Brownian hard disks. We show that long-ranged and long-lived strain-signatures follow a scaling law valid close to the glass transition. For large enough viscosities, the Eshelby-strain pattern is visible even on time scales longer than the structural relaxation time $τ$ and after the shear modulus has relaxed to zero.

cond-mat.soft

Discontinuous shear modulus determines the glass transition temperature

A solid - amorphous or crystalline - is defined by a finite shear modulus while a fluid lacks such. We thus experimentally investigate the elastic properties of a colloidal glass former near the glass transition: spectroscopy of vibrational excitations yields the dispersion relations of longitudinal and transverse phonons in the glassy state. From the long wavelength limit of the dispersion relation we extract the bulk and the shear modulus. As expected, the latter disappear in a fluid and we measure a clearly resolved discontinuous behaviour of the elastic moduli at the glass transition. This not only determines the transition temperature T_G of the system but also directly addresses recent discussions about elasticity during vitrification. We show that low frequency excitations in our system are plane waves such that continuum elasticity theory can be used to describe the macroscopic behaviour.

cond-mat.soft

Kibble-Zurek mechanism in colloidal monolayers

The Kibble-Zurek mechanism describes the evolution of topological defect structures like domain walls, strings, and monopoles when a system is driven through a second order phase transition. The model is used on very different scales like the Higgs field in the early universe or quantum fluids in condensed matter systems. A defect structure naturally arises during cooling if separated regions are too far apart to `communicate' (e.g. about their orientation or phase) due to finite signal velocity. This results in separated domains with different (degenerated) locally broken symmetry. Within this picture we investigate the non-equilibrium dynamics in a condensed matter analogue, a two-dimensional ensemble of colloidal particles. In equilibrium it obeys the so called Kosterlitz-Thouless-Halperin-Nelson-Young (KTHNY) melting scenario with continuous (second-order like) phase transitions. The ensemble is exposed to a set of finite cooling rates covering roughly three orders of magnitude. Along this process, we analyze the defect and domain structure quantitatively via video microscopy and determine the scaling of the corresponding length scales as a function of the cooling rate. We indeed observe the scaling predicted by the Kibble-Zurek mechanism for the KTHNY universality class.

cond-mat.soft

Entropy and Kinetics of Point-Defects in Two-Dimensional Dipolar Crystals

We study in experiment and with computer simulation the free energy and the kinetics of vacancy and interstitial defects in two-dimensional dipolar crystals. The defects appear in different local topologies which we characterize by their point group symmetry; $C_n$ is the n-fold cyclic group and $D_n$ is the dihedral group, including reflections. The frequency of different local topologies is not determined by their almost degenerate energies but dominated by entropy for symmetric configurations. The kinetics of the defects is fully reproduced by a master equation in a multi-state Markov model. In this model, the system is described by the state of the defect and the time evolution is given by transitions occurring with particular rates. These transition rate constants are extracted from experiments and simulations using an optimisation procedure. The good agreement between experiment, simulation and master equation thus provides evidence for the accuracy of the model.

cond-mat.soft

Spontaneous symmetry breaking in 2D: Kibble-Zurek mechanism in temperature quenched colloidal monolayers

The Kibble-Zurek mechanism describes the formation of topological defects during spontaneous symmetry breaking for quite different systems. Shortly after the big bang, the isotropy of the Higgs-field is broken during the expansion and cooling of the universe. Kibble proposed the formation of monopoles, strings, and membranes in the Higgs field since the phase of the symmetry broken field can not switch globally to gain the same value everywhere in space. Zurek pointed out that the same mechanism is relevant for second order phase transitions in condensed matter systems. Every finite cooling rate induces the system to fall out of equilibrium which is due to the critical slowing down of order parameter fluctuations: the correlation time diverges and the symmetry of the system can not change globally but incorporates defects between different domains. Depending on the cooling rate the heterogeneous order parameter pattern are a fingerprint of critical fluctuations. In the present manuscript we show that a monolayer of superparamagnetic colloidal particles is ideally suited to investigate such phenomena. In thermal equilibrium the system undergos continuous phase transitions according KTHNY-theory. If cooled rapidly across the melting temperature the final state is a polycrystal. We show, that the observations can not be explained with nucleation of a supercooled fluid but is compatible with the Kibble-Zurek mechanism.

cond-mat.soft

Specific heat in two-dimensional melting

We report the specific heat $c_N$ around the melting transition(s) of micrometer-sized superparamagnetic particles confined in two dimensions, calculated from fluctuations of positions and internal energy, and corresponding Monte Carlo simulations. Since colloidal systems provide single particle resolution, they offer the unique possibility to compare the experimental temperatures of peak position of $c_N(T)$ and symmetry breaking, respectively. While order parameter correlation functions confirm the Kosterlitz-Thouless-Halperin-Nelson-Young melting scenario where translational and orientational order symmetries are broken at different temperatures with an intermediate so called hexatic phase, we observe a single peak of the specific heat within the hexatic phase, with excellent agreement between experiment and simulation. Thus, the peak is not associated with broken symmetries but can be explained with the total defect density, which correlates with the maximum increase of isolated dislocations. The absence of a latent heat strongly supports the continuous character of both transitions.

cond-mat.soft

Self-organized defect strings in two-dimensional crystals

Using experiments with single particle resolution and computer simulations we study the collective behaviour of multiple vacancies injected into two-dimensional crystals. We find that the defects assemble into linear strings that propagate through the crystal in a succession of rapid one-dimensional gliding phases and rare rotations, during which the direction of motion changes. At both ends, strings are terminated by dislocations with anti-parallel Burgers vectors. By monitoring the separation of the dislocations, we measure their effective interactions with high precision, for the first time beyond spontaneous formation and annihilation, and explain the double-well form of the dislocation interaction in terms of continuum elasticity theory. Our results give a detailed picture of the motion and interaction of dislocations in two dimensions and enhance our understanding of topological defects in two-dimensional nano-materials.

cond-mat.stat-mech

Two-dimensional melting under quenched disorder

We study the influence of quenched disorder on the two-dimensional melting behavior by using both video-microscopy of superparamagnetic colloidal particles and computer simulations of repulsive parallel dipoles. Quenched disorder is provided by pinning a fraction of the particles. We confirm the occurrence of the Kosterlitz-Thouless-Halperin-Nelson-Young scenario with an intermediate hexatic phase. While the fluid-hexatic transition remains largely unaffected by disorder, the hexatic-solid transition shifts towards lower temperatures for increasing disorder resulting in a significantly broadened stability range of the hexatic phase. In addition, we observe spatio-temporal critical(-like) fluctuations consistent with the continuous character of the phase transitions.

cond-mat.soft

Comparison of 2D melting criteria in a colloidal system

We use super-paramagnetic spherical particles which are arranged in a two-dimensional monolayer at a water/air interface to investigate the crystal to liquid phase transition. According to the KTHNY theory a crystal melts in thermal equilibrium by two continuous phase transitions into the isotropic liquid state with an intermediate phase, commonly known as hexatic phase. We verify the significance of several criteria based on dynamical and structural properties to identify the crystal - hexatic and hexatic - isotropic liquid phase transition for the same experimental data of the given setup. Those criteria are the bond orientational correlation function, the Larson-Grier criterion, 2D dynamic Lindemann parameter, the bond-orientational susceptibility, the 2D Hansen-Verlet rule, the Löwen-Palberg-Simon criterion as well as a criterion based on the shape factor of Voronoi cells and Minkowski functionals. For our system with long range repulsion, the bond order correlation function and bond order susceptibility works best to identify the hexatic - isotropic liquid transition and the 2D dynamic Lindemann parameter identifies unambiguously the hexatic - crystalline transition.

cond-mat.soft

Glass elasticity from particle trajectories

Using positional data from video-microscopy of a two-dimensional colloidal system and from simulations of hard discs we determine the wave-vector-dependent normal mode spring constants in the supercooled fluid and glassy state, respectively. The emergence of rigidity and the existence of a displacement field in amorphous solids is clarified. Continuum elastic theory is used in the limit of long wavelengths to analyze the bulk and shear modulus of this amorphous system as a function of temperature. The onset of a finite static shear modulus upon cooling marks the fluid/solid transition. This provides an opportunity to determine the glass transition temperature $T_g$ in an intuitive and precise way.

cond-mat.soft

Ultra-fast quenching of binary colloidal suspensions in an external magnetic field

An ultra-fast quench is applied to binary mixtures of superparamagnetic colloidal particles confined at a two-dimensional water-air interface by a sudden increase of an external magnetic field. This quench realizes a virtually instantaneous cooling which is impossible in molecular systems. Using real-space experiments, the relaxation behavior after the quench is explored. Local crystallites with triangular and square symmetry are formed on different time scales and the correlation peak amplitude of the small particles evolves nonmonotonically in time in agreement with Brownian dynamics computer simulations.

cond-mat.soft