Probing dynamics of dense suspensions: three-dimensional cross-correlation technique

We describe the realization of a novel three-dimensional (3D) cross-correlation scheme, which provides the possibility to measure dynamic structure factors of highly concentrated colloidal samples without contributions of multiply scattered light. The apparatus is easier to align and more compact than the two-colour cross-correlation apparatus, which is commercially available. This should make the 3D cross-correlation set-up more convenient for routine applications, for example in industrial laboratories. We describe the set-up and discuss some special features of the optical components.

Approaching the limits of multiple scattering decorrelation: 3D light-scattering apparatus utilising semiconductor lasers

Light scattering as a function of scattering angle can be regarded as a standard method to investigate the dynamics of dilute colloidal suspensions. Concentrated suspensions, which are of interest if interactions between the particles are to be investigated, usually show strong multiple scattering. Decorrelation of multiple scattered light, which isolates single scattering events at the expense of a reduced signal-to-noise ratio, has been proven to work using the two-colour crosscorrelation scheme.

Enhanced structural correlations accelerate diffusion in charge-stabilized colloidal suspensions

Theoretical calculations for colloidal charge-stabilized and hard sphere suspensions show that hydrodynamic interactions yield a qualitatively different particle concentration dependence of the short-time self-diffusion coefficient. The effect, however, is numerically small and hardly accessible by conventional light scattering experiments. Applying multiple-scattering decorrelation equipment and a careful data analysis we show that the theoretical prediction for charged particles is in agreement with our experimental results from aqueous polystyrene latex suspensions.

Particle Characterization Using Multiple Scattering Decorrelation Methods. Part 1: Standard Latex Particles

Dynamic light scattering by preserved skimmed cow milk: A comparison of two-colour and three-dimensional cross-correlation experiments

We investigate the dynamic light scattering of preserved skimmed cow milk and compare the performance of a standard two-colour (2C) cross-correlation setup with the recently developed three-dimensional (3D) cross-correlation setup. Undiluted milk could only be investigated using the 3D setup because of too low signal-to-noise ratio of the 2C setup. A tenfold diluted milk, however, could be investigated by both setups, and comparable results for the dynamics of the sample were obtained thus demonstrating the equivalence of the decorrelation schemes. On the other hand, we found that the dynamics of the milk is strongly altered upon dilution. This finding elucidates the benefits of the new 3D …

Crystallizing polystyrene microgel colloids

Spherical microgel particles of sufficiently high degree of internal cross-linking and swollen in a good solvent in many respects behave quite similarly to hard-sphere colloids. Due to solvent uptake they can be refractive-index-matched and density-matched in suitable organic solvents. We present preliminary measurements of the crystallization kinetics of 1:10 cross-linked polystyrene microgel particles. We measured Bragg and small-angle light scattering of the solidifying shear melt. Two different scattering patterns, a set of Debye-Scherrer rings and a second ring pattern at small angles could be observed. We check for similarities and differences compared to previously investigated collo…

Effect of uniaxial deformation on the optical scattering losses of a semicrystalline fluorocopolymer.

Both small- and wide-angle light scattering as well as transmission measurements have been used to investigate the optical scattering losses of a vinylidene difluoride–tetrafluoroethylene–hexafluoropropylene copolymer crystallized from the melt. The main origin of the scattering loss is the wide-angle light scattering from the spherulitic superstructure. Uniaxial deformation transforms this structure into a fiber morphology. The attenuation of fibers has been measured for light propagating both parallel and perpendicular to the orientation axis. For both directions, the attenuation decreases with increasing draw ratio. Annealing of the fibers while keeping their ends fixed is an effective m…

Acoustic spectroscopy of aerogel precursors

We investigate the acoustical properties of silica gels, which are precursors in the aerogel production process. These gels exhibit a strong “ringing gel” behavior, that is they emit a characteristic sound if one knocks against the container. We study this sound emission with a very simple spectroscopic technique and observe resonances which are characteristic for natural frequencies of a cylindrical body. From a fit of the experimental frequency positions to calculated values, we determine a sound velocity of c T = 4 m/s for a gel sample with porosity φ = 97.5%. This low sound velocity can only be interpreted as the transverse sound mode predicted by Biot’s theory for sound propagation in …

Three-dimensional dynamic light scattering

Abstract We describe the employment of a novel light-scattering scheme for the decorrelation of multiple scattering in strongly turbid samples. The three-dimensional scheme, which has been proposed already theoretically, shows certain advantages compared with the two-colour apparatus, which is commercially available. We describe our set-up in detail; features are the use of modern semiconductor laser diodes and contemporary single-mode fibre receivers. We show experimentally that the optimal signal-to-noise ratio (or intercept) β opt = 0.20, which is obtainable with our set-up, can be quantitatively calculated from the measured uncertainties in the alignment. In particular, we give a detail…

Particle characterization using multiple scattering decorrelation methods: hard-sphere model system

Applying static light scattering experiments, we characterize colloidal particles that are used as model hard-sphere systems in experiments investigating their crystallization kinetics. The particles comprise of a compact core of poly(methyl methacrylate) and short polymer hairs grafted onto the surface. We use a contrast variation procedure to determine the refractive index variation within the particles and observe that one component of the binary mixture used as a solvent penetrates the particles and masks completely the small polymer hairs. Making use of the determined refractive index variation, we obtain the average particle radius and its polydispersity from measurements of the parti…

Observation of Oriented Close-Packed Lattice Planes in Polycrystalline Hard-Sphere Solids.

We report time-resolved Bragg scattering experiments on solidifying colloidal suspensions of hard spheres. The polar angle-averaged, integrated intensity of the (111) and (311) reflections show a transient, two-step behavior below melting, which depends in a complex way on the volume fraction and is not present for (200) or (220). Detailed analysis of the full two-dimensional scattering pattern reveals intensity maxima of sixfold symmetry close to the position of the (111) and (311) Debye-Scherrer rings. These can be explained assuming oriented crystals with close-packed planes parallel to the container walls. We show that the observed temporal behavior is due to competing homogeneous and h…

Solidification kinetics of hard-sphere colloidal suspensions

We investigate the solidification dynamics of hard-sphere colloidal suspensions applying simultaneously small-angle and Bragg light scattering. These experiments allow a consistent picture of nucleation and crystal growth on the level of large-scale density fluctuations and of density fluctuations on the level of individual crystallites. We observe a temporally almost constant nucleation rate after an induction time that decreases with supersaturation. The classical expectation for the nucleation rate density as a function of supersaturation is in accordance with our data. We investigate the validity of the Wilson—Frenkel growth law for hard-sphere systems, which also fits our data satisfac…

Suppression of the speckle noise in solid polymer samples: a light scattering study

The speckle effect disturbs the measurement of spatial correlation functions in solid polymer samples by light scattering. To be able to extract the desired correlations from the measurements, the speckle noise must be suppressed. This is possible by moving the sample during the measurement. In this paper we demonstrate that a sufficient reduction of speckle contrast can be achieved even in samples of restricted dimensions or with a preferential direction.