3D functional ultrasound imaging of pigeons.

Recent advances in ultrasound Doppler imaging have facilitated the technique of functional ultrasound (fUS) which enables visualization of brain-activity due to neurovascular coupling. As of yet, this technique has been applied to rodents as well as to human subjects during awake craniotomy surgery and human newborns. Here we demonstrate the first successful fUS studies on awake pigeons subjected to auditory and visual stimulation. To allow successful fUS on pigeons we improved the temporal resolution of fUS up to 20,000 frames per second with real-time visualization and continuous recording. We show that this gain in temporal resolution significantly increases the sensitivity for detecting small fluctuations in cerebral blood flow and volume which may reflect increased local neural activity. Through this increased sensitivity we were able to capture the elaborate 3D neural activity pattern evoked by a complex stimulation pattern, such as a moving light source. By pushing the limits of fUS further, we have reaffirmed the enormous potential of this technique as a new standard in functional brain imaging with the capacity to unravel unknown, stimulus related hemodynamics with excellent spatiotemporal resolution with a wide field of view.

Pulse wave analysis with diffusing-wave spectroscopy.

Hypertension is a major risk factor for cardiovascular disease and thus at the origin of many deaths by e.g. heart attack or stroke. Hypertension is caused by many factors including an increase in arterial stiffness which leads to changes in pulse wave velocity and wave reflections. Those often result in an increased left ventricular load which may result in heart failure as well as an increased pulsatile pressure in the microcirculation l to damage to blood vessels. In order to specifically treat the different causes of hypertension it is desirable to perform a pulse wave analysis as a complement to measurements of systolic and diastolic pressure by brachial cuff sphygmomanometry. Here we show that Diffusing Wave Spectroscopy, a novel non-invasive portable tool, is able to monitor blood flow changes with a high temporal resolution. The measured pulse travel times give detailed information of the pulse wave blood flow profile.

Free-Standing Photonic Glasses Fabricated in a Centrifugal Field.

One efficient method to obtain disordered colloidal packing is to reduce the stability of colloidal particles by adding electrolytes to the colloidal dispersions. But the correct amount of additional electrolytes must be found empirically. Here, the effect of CaCl2 on polystyrene colloidal dispersions is studied, and a link between the amount of CaCl2 and the corresponding glassy colloidal structure is quantitatively built. A threshold concentration of CaCl2 is found by dynamic light scattering. When exceeding this threshold, different nanoparticle oligomers are observed in the dispersions by analytical ultracentrifugation. The second objective is to achieve free-standing samples, which is required for many optical measurements. A universal method is established, using a centrifugal field to produce robust samples by polymerizing coassembled hydrophilic monomers to form a network, which traps the glassy colloidal structures. Photon time of flight measurements shows that the CaCl2 concentration threshold should not be exceeded. Otherwise an optical shortcut may take place. Thus, the work provides a feasible universal route to prepare macroscopic free-standing photonic glasses from electrostatically stabilized nanoparticles, suitable for further optical investigation.

Magneto-Adaptive Surfactants Showing Anti-Curie Behavior and Tunable Surface Tension as Porogens for Mesoporous Particles with 12-Fold Symmetry.

Gaining external control over self-organization is of vital importance for future smart materials. Surfactants are extremely valuable for the synthesis of diverse nanomaterials. Their self-assembly is dictated by microphase separation, the hydrophobic effect, and head-group repulsion. It is desirable to supplement surfactants with an added mode of long-range and directional interaction. Magnetic forces are ideal, as they are not shielded in water. We report on surfactants with heads containing tightly bound transition-metal centers. The magnetic moment of the head was varied systematically while keeping shape and charge constant. Changes in the magnetic moment of the head led to notable differences in surface tension, aggregate size, and contact angle, which could also be altered by an external magnetic field. The most astonishing result was that the use of magnetic surfactants as structure-directing agents enabled the formation of porous solids with 12-fold rotational symmetry.

Mermin-Wagner fluctuations in 2D amorphous solids.

In a recent commentary, J. M. Kosterlitz described how D. Thouless and he got motivated to investigate melting and suprafluidity in two dimensions [Kosterlitz JM (2016) J Phys Condens Matter 28:481001]. It was due to 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). 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 in the sense that the mean squared displacement of atoms is not limited. Comparing experimental data from 3D and 2D amorphous solids with 2D crystals, we disentangle Mermin-Wagner fluctuations from glassy structural relaxations. Furthermore, we demonstrate with computer simulations the logarithmic increase of displacements with system size: Periodicity is not a requirement for Mermin-Wagner fluctuations, which conserve the homogeneity of space on long scales.

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 lack of causality results in separated domains with different (degenerated) locally broken symmetry. Within this picture, we investigate the nonequilibrium dynamics in a condensed matter analog, a 2D 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.

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; Cn is the n-fold cyclic group and Dn is the dihedral group, including reflections. The frequency of different local topologies is not determined by their almost degenerate energies but is dominated by entropy for symmetric configurations. The kinetics of the defects is fully reproduced by a master equation in a multistate 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 optimization procedure. The good agreement between experiment, simulation, and master equation thus provides evidence for the accuracy of the model.

Grain-boundary-induced melting in quenched polycrystalline monolayers.

Melting in two dimensions can successfully be explained with the Kosterlitz-Thouless-Halperin-Nelson-Young (KTHNY) scenario which describes the formation of the high-symmetry phase with the thermal activation of topological defects within an (ideally) infinite monodomain. With all state variables being well defined, it should hold also as freezing scenario where oppositely charged topological defects annihilate. The Kibble-Zurek mechanism, on the other hand, shows that spontaneous symmetry breaking alongside a continuous phase transition cannot support an infinite monodomain but leads to polycrystallinity. For any nonzero cooling rate, critical fluctuations will be frozen out in the vicinity of the transition temperature. This leads to domains with different director of the broken symmetry, separated by a defect structure, e.g., grain boundaries in crystalline systems. After instantaneously quenching a colloidal monolayer from a polycrystalline to the isotropic fluid state, we show that such grain boundaries increase the probability for the formation of dislocations. In addition, we determine the temporal decay of defect core energies during the first few Brownian times after the quench. Despite the fact that the KTHNY scenario describes a continuous phase transition and phase equilibrium does not exist, melting in polycrystalline samples starts at grain boundaries similar to first-order phase transitions.

Specific heat in two-dimensional melting.

We report the specific heat cN 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 the peak position of cN(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.

Two-dimensional melting under quenched disorder.

We study the influence of quenched disorder on the two-dimensional melting behavior of superparamagnetic colloidal particles, using both video microscopy and computer simulations of repulsive parallel dipoles. Quenched disorder is introduced by pinning a fraction of the particles to an underlying substrate. We confirm the occurrence of the Kosterlitz-Thouless-Halperin-Nelson-Young scenario and observe an intermediate hexatic phase. While the fluid-hexatic transition remains largely unaffected by disorder, the hexatic-solid transition shifts to lower temperatures with increasing disorder. This results in a significantly broadened stability range of the hexatic phase. In addition, we observe spatiotemporal critical(like) fluctuations, which are consistent with the continuous character of the phase transitions. Characteristics of first-order transitions are not observed.

Self-organized defect strings in two-dimensional crystals.

Using experiments with single-particle resolution and computer simulations we study the collective behavior of multiple vacancies injected into two-dimensional crystals. We find that the defects assemble into linear strings, terminated by dislocations with antiparallel Burgers vectors. We show that these defect strings propagate through the crystal in a succession of rapid one-dimensional gliding and rare rotations. While the rotation rate decreases exponentially with the number of defects in the string, the diffusion constant is constant for large strings. By monitoring the separation of the dislocations at the end points, we measure their effective interactions with high precision beyond their spontaneous formation and annihilation, and we explain the double-well form of the dislocation interaction in terms of continuum elasticity theory.

Fluctuations of orientational order and clustering in a two-dimensional colloidal system under quenched disorder.

Using both video microscopy of superparamagnetic colloidal particles confined in two dimensions and corresponding computer simulations of repulsive parallel dipoles, we study the formation of fluctuating orientational clusters and topological defects in the context of the KTHNY-like melting scenario under quenched disorder. We analyze cluster densities, average cluster sizes, and the population of noncluster particles, as well as the development of defects, as a function of the system temperature and disorder strength. In addition, the probability distribution of clustering and orientational order is presented. We find that the well-known disorder-induced widening of the hexatic phase can be traced back to the distinct development characteristics of clusters and defects along the melting transitions from the solid phase to the hexatic phase to the isotropic fluid.

Glass elasticity from particle trajectories.

Using positional data from video microscopy of a two-dimensional colloidal system and from simulations of hard disks, we determine the wave-vector-dependent elastic dispersion relations in glass. The emergence of rigidity based on the existence of a well defined displacement field in amorphous solids is demonstrated. Continuum elastic theory is recovered in the limit of long wavelengths which provides the glass elastic shear and bulk modulus as a function of temperature. The onset of a finite static shear modulus upon cooling marks the fluid-glass transition in an intuitive and unique way.

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 the 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 transitions for the same experimental data of the given setup. The criteria are the bond orientational correlation function, the Larson-Grier criterion, the 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 work best to identify the hexatic-isotropic liquid transition and the 2D dynamic Lindemann parameter identifies unambiguously the hexatic-crystalline transition.

Melting of crystals in two dimensions.

While the melting of crystals is in general not understood in detail on a microscopic scale, there is a microscopic theory for a class of two-dimensional crystals, which is based on the formation and unbinding of topological defects. Herein, we review experimental work on a colloidal two-dimensional model system with tunable interactions that has given the first conclusive evidence for the validity of this theory on a microscopic level. Furthermore, we show how the mechanism of melting depends on the particle interaction and that a strong anisotropy of the interaction leads to a changed melting scenario.

Ultrafast quenching of binary colloidal suspensions in an external magnetic field.

An ultrafast 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.

Observation of Anderson localization of light in three dimensions.

Using time-resolved transmission measurements, we have found indications of Anderson localization of light in bulk three-dimensional systems. The observed deviation from classical diffusion is in good accord with theoretical predictions of localization and cannot be explained by absorption or experimental artifacts such as stratification, fluorescence, or background illumination. Moreover, we show that in our samples the control parameter is given by the mean free path times the wavenumber as required by the Ioffe-Regel criterion. This is in contrast to quasi-one-dimensional systems that were studied with microwaves. There, the control parameter is related to the number of modes inside a waveguide, and deviations from classical diffusion are possible due to a small number of modes.

Partial clustering in binary two-dimensional colloidal suspensions.

Strongly interacting binary mixtures of superparamagnetic colloidal particles confined to a two-dimensional water-air interface are examined by theory, computer simulation, and experiment. The mixture exhibits a partial clustering in equilibrium: in the voids of the matrix of unclustered big particles, the small particles form subclusters with a spongelike topology which is accompanied by a characteristic small-wave vector peak in the small-small structure factor. This partial clustering is a general phenomenon occurring for strongly coupled negatively nonadditive mixtures.

Reduced transport velocity of multiply scattered light due to resonant scattering.

The transport properties of photons traveling through random media are of great fundamental and applied importance. For instance the dwell time due to resonant Mie scattering can lead to a significant reduction in transport velocity. Here, we have measured directly the energy-transport velocity of photons in strongly scattering media using a combination of time resolved transmission, measuring the diffusion coefficient, and angular resolved backscattering, yielding the transport mean free path. We find that the transport velocity is strongly reduced when the effective diameter of the scattering particles is a multiple of half the wavelength. This is consistent with the occurrence of resonant Mie scattering in the samples. We compare our data to previous theoretical calculations of the transport velocity as a function of scatterer size.

Observation of the critical regime near Anderson localization of light.

The transition from diffusive transport to localization of waves should occur for any type of classical or quantum wave in any media as long as the wavelength becomes comparable to the transport mean free path l*. The signatures of localization and those of absorption, or bound states, can, however, be similar, such that an unequivocal proof of the existence of wave localization in disordered bulk materials is still lacking. Here we present time resolved measurements of light transport through strongly scattering samples with kl* values as low as 2.5. In transmission, we observe deviations from diffusion which cannot be explained by absorption, sample geometry, or reduction in transport velocity. Furthermore, the deviations from classical diffusion increase strongly with decreasing l* as expected for a phase transition. This constitutes an experimental realization of the critical regime in the approach to Anderson localization.