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Atomic force microscopy (AFM) is a powerful technique for imaging molecules, macromolecular complexes, and nanoparticles with nanometer-resolution. However, AFM images are distorted by the shape of the tip used. These distortions can be corrected if the tip shape can be determined by scanning a sample with features sharper than the tip and higher than the object of interest. Here we present a 3D DNA origami structure as fiducial for tip reconstruction and image correction. Our fiducial is stable under a broad range of conditions and has sharp steps at different heights that enable reliable tip reconstruction from as few as ten fiducials. The DNA origami is readily co-deposited with biological and non-biological samples, achieves higher precision for the tip apex than polycrystalline samples, and dramatically improves the accuracy of the lateral dimensions determined from the images. Our fiducial thus enables accurate and precise AFM imaging for a broad range of applications.

We report methods to synthesize sub-micron- and micron-sized patchy silica particles with fluorescently labeled hemispherical titania protrusions, as well as routes to efficiently characterize these particles and self-assemble these particles into non-close-packed structures. The synthesis methods expand upon earlier work in the literature, in which silica particles packed in a colloidal crystal were surface-patterned with a silane coupling agent. Here, hemispherical amorphous titania protrusions were successfully labeled with fluorescent dyes, allowing for imaging by confocal microscopy and super-resolution techniques. Confocal microscopy was exploited to experimentally determine the numbers of protrusions per particle over large numbers of particles for good statistical significance, and these distributions were compared to simulations predicting the number of patches as a function of core particle polydispersity and maximum separation between the particle surfaces. We self-assembled these patchy particles into open percolating gel networks by exploiting solvophobic attractions between the protrusions.

Extending the toolbox from mono- to bimetallic catalysts is key in realizing efficient chemical processes. Traditionally, the performance of bimetallic catalysts featuring one active and one selective metal is optimized by varying the metal composition, often resulting in a compromise between the catalytic properties of the two metals. Here we show that by designing the atomic distribution of bimetallic Au-Pd nanocatalysts, we obtain a synergistic catalytic performance in the industrially relevant selective hydrogenation of butadiene. Our single crystalline Au-core Pd-shell nanorods were up to 50 times more active than their alloyed and monometallic counterparts, while retaining high selectivity. We find a shell thickness dependent catalytic activity, indicating that not only the nature of the surface but also several sub-surface layers play a crucial role in the catalytic performance, and rationalize this finding using density-functional-theory calculations. Our results open up a novel avenue for the structural design of bimetallic catalysts.

Extending the toolbox from mono- to bimetallic catalysts is key in realizing efficient chemical processes

The influence of geometry on the local and global packing of particles is important to many fundamental and applied research themes, such as the structure and stability of liquids, crystals and glasses. Here we show by experiments and simulations that a binary mixture of hard-sphere-like nanoparticles crystallizing into a MgZn(2)Laves phase in bulk spontaneously forms icosahedral clusters in slowly drying droplets. Using advanced electron tomography, we are able to obtain the real-space coordinates of all the spheres in the icosahedral clusters of up to about 10,000 particles. The local structure of 70-80% of the particles became similar to that of the MgCu(2)Laves phase. These observations are important for photonic applications. In addition, we observed in simulations that the icosahedral clusters nucleated away from the spherical boundary, which is distinctly different from that of the single species clusters. Our findings open the way for particle-level studies of nucleation and growth of icosahedral clusters, and of binary crystallization. The authors investigate out-of-equilibrium crystallization of a binary mixture of sphere-like nanoparticles in small droplets. They observe the spontaneous formation of an icosahedral structure with stable MgCu(2)phases, which are promising for photonic applications.

Chemotactic interactions are ubiquitous in nature and can lead to non-reciprocal and complex emergent behaviour in multibody systems. However, developing synthetic, inanimate embodiments of a chemomechanical framework to generate non-reciprocal interactions of tunable strength and directionality has been challenging. Here we show how chemotactic signalling between microscale oil droplets of different chemistries in micellar surfactant solutions can result in predator-prey-like non-reciprocal chasing interactions. The interactions and dynamic self-organization result from the net directional, micelle-mediated transport of oil between emulsion droplets of differing composition and are powered by the free energy of mixing. We systematically elucidated chemical design rules to tune the interactions between droplets by varying the oil and surfactant chemical structure and concentration. Through the integration of experiment and simulation, we also investigated the active behaviour and dynamic reorganization of multidroplet clusters. Our findings demonstrate how chemically minimal systems can be designed with controllable, non-reciprocal chemotactic interactions to generate emergent self-organization and collective behaviours reminiscent of biological systems.

We studied the formation of supraparticles from nanocrystals confined in slowly evaporating oil droplets in an oil-in-water emulsion. The nanocrystals consist of an FeO core, a CoFe2O4 shell, and oleate capping ligands, with an overall diameter of 12.5 nm. We performed in situ small- and wide-angle X-ray scattering experiments during the entire period of solvent evaporation and colloidal crystallization. We observed a slow increase in the volume fraction of nanocrystals inside the oil droplets up to 20%, at which a sudden crystallization occurs. Our computer simulations show that crystallization at such a low volume fraction is only possible if attractive interactions between colloidal nanocrystals are taken into account in the model as well. The spherical supraparticles have a diameter of about 700 nm and consist of a few crystalline face-centered cubic domains. Nanocrystal supraparticles bear importance for magnetic and optoelectronic applications, such as color tunable biolabels, color tunable phosphors in LEDs, and miniaturized lasers.

Assembling binary mixtures of nanoparticles into crystals, gives rise to collective properties depending on the crystal structure and the individual properties of both species. However, quantitative 3D real-space analysis of binary colloidal crystals with a thickness of more than 10 layers of particles has rarely been performed. Here we demonstrate that an excess of one species in the binary nanoparticle mixture suppresses the formation of icosahedral order in the self-assembly in droplets, allowing the study of bulk-like binary crystal structures with a spherical morphology also called supraparticles. As example of the approach, we show single-particle level analysis of over 50 layers of Laves phase binary crystals of hard-sphere-like nanoparticles using electron tomography. We observe a crystalline lattice composed of a random mixture of the Laves phases. The number ratio of the binary species in the crystal lattice matches that of a perfect Laves crystal. Our methodology can be applied to study the structure of a broad range of binary crystals, giving insights into the structure formation mechanisms and structure-property relations of nanomaterials., 3D real-space analysis of thick nanoparticle crystals is non-trivial. Here, the authors demonstrate the structural analysis of a bulk-like Laves phase by imaging an off-stoichiometric binary mixture of hard-sphere-like nanoparticles in spherical confinement by electron tomography, enabling defect analysis on the single-particle level.

Cellulose microfibrils (CMFs) are an important nanoscale building block in many novel biobased functional materials. The spatial nano- and microscale organization of the CMFs is a crucial factor for defining the properties of these materials. Here, we report for the first time a direct three-dimensional (3D) real-space analysis of individual CMFs and their networks formed after ultrahigh-shear-induced transient deagglomeration and self-assembly in a solvent. Using point-scanning confocal microscopy combined with tracking the centerlines of the fibrils and their junctions by a stretching open active contours method, we reveal that dispersions of the native CMFs assemble into highly heterogeneous networks of individual fibrils and bundles. The average network mesh size decreases with increasing CMF volume fraction. The cross-sectional width and the average length between the twists in the ribbon-shaped CMFs are directly determined and compared well with that of fibrils in the dried state. Finally, the generality of the fluorescent labeling and imaging approach on other CMF sources is illustrated. The unique ability to quantify in situ the multiscale structure in CMF dispersions provides a powerful tool for the correlation of process-structure-property relationship in cellulose-containing composites and dispersions.

Nanoparticle assemblies can be investigated in 3 dimensions using electron tomography. However, it is not straightforward to obtain quantitative information such as the number of particles or their relative position. This becomes particularly difficult when the number of particles increases. We propose a novel approach in which prior information on the shape of the individual particles is exploited. It improves the quality of the reconstruction of these complex assemblies significantly. Moreover, this quantitative Sparse Sphere Reconstruction approach yields directly the number of particles and their position as an output of the reconstruction technique, enabling a detailed 3D analysis of assemblies with as many as 10 000 particles. The approach can also be used to reconstruct objects based on a very limited number of projections, which opens up possibilities to investigate beam sensitive assemblies where previous reconstructions with the available electron tomography techniques failed.

The search for new functional soft materials with precise and reconfigurable structures at the nano and meso-scale is a major challenge as well as objective of the current science. Patchy colloids of different shapes and functionalities are considered important new building blocks of a bottom-up approach towards rational design of new soft materials largely governed by anisotropic interactions. Herein, we investigate the self-assembly, growth of hierarchical microstructures and aging dynamics of 2D nano-platelets of two different aspect ratios (Laponite ~25 and Montmorillonite ~250) which form gels with different porosity that is achieved by tuning their mixing ratios. Qualitative in situ real-space studies are carried out, including fluorescent confocal microscopy imaging of the bicontinuous gelation process or final states, which provides dynamic visualization of the self-organization. The bicontinuous gels exhibit a foam-like morphology having pores of a few micrometers in size that can be tuned by varying the mixing ratio of nanoplatelets. It is shown that this new class of clay gels has unique and tunable physical properties that will find potential applications in the development of low cost lithium ion batteries, nanocomposites and nuclear waste management.

Janus nanoparticles (NPs) often referred to as nanosized analogs of molecular surfactants are amphiphilic structures with potential applications in materials science, biomedicine, and catalysis, and their synthesis and self-assembly into complex architectures remain challenging. Here, we demonstrate the preparation of Janus heterodimers via asymmetric functionalization of Fe

Anisotropic bimetallic nanoparticles are promising candidates for plasmonic and catalytic applications. Their catalytic performance and plasmonic properties are closely linked to the distribution of the two metals, which can change during applications in which the particles are exposed to heat. Due to this fact, correlating the thermal stability of complex heterogeneous nanoparticles to their microstructural properties is of high interest for the practical applications of such materials. Here, we employ quantitative electron tomography in high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) mode to measure the 3D elemental diffusion dynamics in individual anisotropic Au–Ag nanoparticles upon heating in situ. This approach allows us to study the elemental redistribution in complex, asymmetric nanoparticles on a single particle level, which has been inaccessible to other techniques so far. In this work, we apply the proposed method to compare the alloying dynamics of Au–Ag nanoparticles with different shapes and compositions and find that the shape of the nanoparticle does not exhibit a significant effect on the alloying speed whereas the composition does. Finally, comparing the experimental results to diffusion simulations allows us to estimate the diffusion coefficients of the metals for individual nanoparticles.

The rapid development of nanomaterials with unique size-tunable properties forms the basis for a variety of new applications, including temperature sensing. Luminescent nanoparticles (NPs) have demonstrated potential as sensitive nanothermometers, especially in biological systems. Their small size offers the possibility of mapping temperature profiles with high spatial resolution. The temperature range is however limited, which prevents use in high-temperature applications such as, for example, nanoelectronics, thermal barrier coatings, and chemical reactors. In this work, we extend the temperature range for nanothermometry beyond 900 K using silica-coated NaYF4 nanoparticles doped with the lanthanide ions Yb3+ and Er3+. Monodisperse ∼20 nm NaYF4:Yb,Er nanocrystals were coated with a ∼10 nm silica shell. Upon excitation with infrared radiation, bright green upconversion (UC) emission is observed. From the intensity ratio between 2H11/2 and 4S3/2 UC emission lines at 520 and 550 nm, respectively, the temperature can be determined up to at least 900 K with an accuracy of 1–5 K for silica-coated NPs. For bare NaYF4:Yb,Er NPs, the particles degrade above 600 K. Repeated thermal cycling experiments demonstrate the high durability and reproducibility of the silica-coated nanocrystals as temperature probes without any loss of performance. The present results open avenues for the development of a new class of highly stable nanoprobes by applying a silica coating around a wide variety of lanthanide-doped NPs.

We performed single particle deformation experiments on silica-coated gold nanorods under femtosecond (fs) illumination. Changes in the particle shape were analyzed by electron microscopy and associated changes in the plasmon resonance by electron energy loss spectroscopy. Silica-coated rods were found to be more stable compared to uncoated rods but could still be deformed via an intermediate bullet-like shape for silica shell thicknesses of 14 nm. Changes in the size ratio of the rods after fs-illumination resulted in blue-shifting of the longitudinal plasmon resonances. Two-dimensional spatial mapping of the plasmon resonances revealed that the flat side of the bullet-like particles showed a less pronounced longitudinal plasmonic electric field enhancement. These findings were confirmed by finite-difference time-domain (FDTD) simulations. Furthermore, at higher laser fluences size reduction of the particles was found as well as for particles that were not completely deformed yet.

Colloidal particles with site-specific directional interactions, so called “patchy particles”, are promising candidates for bottom-up assembly routes towards complex structures with rationally designed properties. Here we present an experimental realization of patchy colloidal particles based on material independent depletion interaction and surface roughness. Curved, smooth patches on rough colloids are shown to be exclusively attractive due to their different overlap volumes. We discuss in detail the case of colloids with one patch that serves as a model for molecular surfactants both with respect to their geometry and their interactions. These one-patch particles assemble into clusters that resemble surfactant micelles with the smooth and attractive sides of the colloids located at the interior. We term these clusters “colloidal micelles”. Direct Monte Carlo simulations starting from a homogeneous state give rise to cluster size distributions that are in good agreement with those found in experiments. Important differences with surfactant micelles originate from the colloidal character of our model system and are investigated by simulations and addressed theoretically. Our new “patchy” model system opens up the possibility for self-assembly studies into finite-sized superstructures as well as crystals with as of yet inaccessible structures.

The catalytic performance and optical properties of bimetallic nanoparticles critically depend on the atomic distribution of the two metals in the nanoparticles. However, at elevated temperatures, during light-induced heating, or during catalysis, atomic redistribution can occur. Measuring such metal redistribution in situ is challenging, and a single experimental technique does not suffice. Furthermore, the availability of a well-defined nanoparticle system has been an obstacle for a systematic investigation of the key factors governing the atomic redistribution. In this study, we follow metal redistribution in precisely tunable, single-crystalline Au-core, Ag-shell nanorods in situ, both at a single particle and an ensemble-averaged level, by combining in situ transmission electron spectroscopy with in situ extended X-ray absorption fine structure validated by ex situ measurements. We show that the kinetics of atomic redistribution in Au-Ag nanoparticles depend on the metal composition and particle volume, such that a higher Ag content or a larger particle size led to significantly slower metal redistribution. We developed a simple theoretical model based on Fick's first law that can correctly predict the composition- and size-dependent alloying behavior in Au-Ag nanoparticles, as observed experimentally.

We describe a general one-pot method for coating colloidal particles with amorphous titania. Various colloidal particles such as silica particles, large silver colloids, gibbsite platelets, and polystyrene spheres were successfully coated with a titania shell. Although there are several ways of coating different particles with titania in the literature, each of these methods is applicable to only one type of material. The present method is especially useful for giving the opportunity to cover many types of colloidal particles with titania and forgoes the use of a coupling agent or a precoating step. We can produce particles with a smooth titania layer of tunable thickness. The monodispersity, which improves during particle growth, and the high refractive index of titania make these particles potential candidates for photonic crystal applications. We also describe various ways of fabricating hollow titania shells, which have been intensively studied in the literature for their applications in electronics, catalysis, separations, and diagnostics. Note that our method initially produces amorphous shells on the particles, but these can be easily turned into crystalline titania by a calcination step. We also find that the growth of titania is a surface-reaction-limited process.

The sedimentation of an initially inhomogeneous distribution of hard-sphere colloids confined in a slit is simulated using the multi-particle collision dynamics scheme which takes into account hydrodynamic interactions mediated by the solvent. This system is an example for soft matter driven out of equilibrium where various length and time scales are involved. The initial laterally homogeneous density profiles exhibit a hydrodynamic Rayleigh-Taylor-like instability. Solvent backflow effects lead to an intricate non-linear behaviour which is analyzed via the solvent flow field and the colloidal velocity correlation function. Our simulation data are in good agreement with real-space microscopy experiments.

2009 WILEY-VCH Verlag Gmb Microscopic ‘colloidal’ particles can spontaneously organize into larger-scale structures, making them important as condensedmatter model systems and advanced materials. Nowadays, one can often predict what structure is needed to obtain certain material properties; the challenge is to experimentally realize the, often complex, particle interactions that lead to those structures. External fields provide one route. Uniaxial electric and magnetic fields are commonly used to induce dipolar interactions, while multi-axial fields bear promise for higher complexity of the interactions. Here, we focus on a biaxial electric field, generated by applying a high-frequency 2D field vector with a randomized orientation, and study in detail how the resulting ‘inverted’ dipolar interactions affect the colloidal self-assembly process. We find that the particles reproducibly form a (most likely non-equilibrium) structure of hexagonal ‘sheets’, which we can make permanent by thermal annealing. Moreover, we can rapidly switch the suspension structure from isotropic, to one-dimensional ‘strings’ and two-dimensional ‘sheets’. This is interesting for applications, because the sample spanning sheets make the suspension properties strongly anisotropic and can dramatically increase the viscosity and thermal conductivity. While the fairly simple inverted dipolar interaction already gives structures that are rather different from those seen in uniaxial fields, our approach could easily be extended to other, more complex interaction potentials as well, by choosing different time-varying functions on the electrodes. For decades, colloidal studies havemostly been concerned with particles with straightforward shapes and simple, mainly isotropic, interactions. This sets certain bounds to their applicability as models of atomic/molecular phase behavior and the number of structures that can be obtained through self-assembly. However, advances in synthesis and chemical modification have recently led to new particle shapes and interaction forms, while external electric or magnetic fields can be used to induce new interactions in existing systems. A major advantage of the latter approach is that the interactions are reversible and that it does not require complicated chemistry. Interestingly, the relatively simple anisotropic dipolar interaction in a uniaxial field already gives rise to several new phases, like body-centered-tetragonal crystals. Recently, Martin et al. reported for granular materials how rotatingmulti-axial fields can open up still another range of novel particle interactions. They derived that in a rotating biaxial field the particles experience the following time-averaged interaction (here given for an electric field, neglecting higher-order multipole contributions; this is a reasonable approximation for the suspensions used in this report)

Shear-induced melting and crystallization were investigated by confocal microscopy in concentrated colloidal suspensions of hard-sphere-like particles. Both silica and polymethylmethacrylate suspensions were sheared with a constant rate in either a countertranslating parallel plate shear cell or a counterrotating cone-plate shear cell. These instruments make it possible to track particles undergoing shear for extended periods of time in a plane of zero velocity. Although on large scales, the flow profile deviated from linearity, the crystal flowed in an aligned sliding layer structure at low shear rates. Higher shear rates caused the crystal to shear melt, but, contrary to expectations, the transition was not sudden. Instead, although the overall order decreased with shear rate, this was due to an increase in the nucleation of localized domains that temporarily lost and regained their ordered structure. Even at shear rates that were considered to have melted the crystal as a whole, ordered regions kept showing up at times, giving rise to very large fluctuations in 2D bond-orientational order parameters. Low shear rates induced initially disordered suspensions to crystallize. This time, the order parameter increased gradually in time without large fluctuations, indicating that shear-induced crystallization of hard spheres does not proceed via a nucleation and growth mechanism. We conclude that the dynamics of melting and crystallization under shear differ dramatically from their counterparts in quiescent suspensions.

We describe a novel method to synthesize colloidal particles with an eccentric core−shell structure. Titania−silica core−shell particles were synthesized by silica coating of porous titania particles under Stober (Stober et al. J. Colloid Interface Sci. 1968, 26, 62) conditions. We can control access of silica to the pores in the titania, allowing us to produce either core−shell or composite particles. Calcination of the core−shell particles gives unique eccentric core−shell structures, as a result of extensive shrinkage of the highly porous titania core with respect to the silica shell. However, when the titania particles are silica treated prior to drying they result in composite titania−silica spheres, where two materials are mixed uniformly. These spheres are interesting for catalysis, (switchable) photonic crystal applications, optical tweezing, and new titiana based materials. We demonstrate photocatalytic activity of the eccentric spheres where the silica layer acts as a size selective membrane.

Core-shell polystyrene-silica spheres with diameters of 800 nm and 1.9 microm were synthesized by soap-free emulsion and dispersion polymerization of the polystyrene core, respectively. The polystyrene spheres were used as templates for the synthesis of silica shells of tunable thickness employing the Stöber method [Graf et al. Langmuir 2003, 19, 6693]. The polystyrene template was removed by thermal decomposition at 500 degrees C, resulting in smooth silica shells of well-defined thickness (15-70 nm). The elastic response of these hollow spheres was probed by atomic force microscopy (AFM). A point load was applied to the particle surface through a sharp AFM tip, and successively increased until the shell broke. In agreement with the predictions of shell theory, for small deformations the deformation increased linearly with applied force. The Young's modulus (18 +/- 6 GPa) was about 4 times smaller than that of fused silica [Adachi and Sakka J. Mater. Sci. 1990, 25, 4732] but identical to that of bulk silica spheres (800 nm) synthesized by the Stöber method, indicating that it yields silica of lower density. The minimum force needed to irreversibly deform (buckle) the shell increased quadratically with shell thickness.

A facile and flexible synthesis for colloidal molecules with well-controlled shape and tunable patchiness is presented. Cross-linked polystyrene spheres with a liquid protrusion were found to assemble into colloidal molecules by coalescence of the liquid protrusions. Similarly, cross-linked poly(methyl methacrylate) particles carrying a wetting layer assembled into colloidal molecules by coalescence of the wetting layer. Driven by surface energy, a liquid droplet on which the solid spheres are attached is formed. Subsequent polymerization of the liquid yields a wide variety of colloidal molecules as well as colloidosomes with tunable patchiness. Precise control over the topology of the particles has been achieved by changing the amount and nature of the swelling monomer as well as the wetting angle between the liquid and the seed particles. The overall cluster size can be controlled by the seed size as well as the swelling ratio. Use of different swelling monomers and/or particles allows for chemical diversity of the patches and the center. For low swelling ratios assemblies of small numbers of seeds resemble clusters that minimize the second moment of the mass distribution. Assemblies comprised of a large number of colloids are similar to colloidosomes exhibiting elastic strain relief by scar formation.

In this work, we show strong experimental evidence in favor of a proposed incorporation mechanism of hydrophobic semiconductor nanocrystals (or quantum dots, QDs) in monodisperse silica spheres (diameter ∼35 nm) by a water-in-oil (W/O) reverse microemulsion synthesis. Fluorescence spectroscopy is used to investigate the rapid ligand exchange that takes place at the QD surface upon addition of the various synthesis reactants. It is found that hydrolyzed TEOS has a high affinity for the QD surface and replaces the hydrophobic amine ligands, which enables the transfer of the QDs to the hydrophilic interior of the micelles where silica growth takes place. By hindering the ligand exchange using stronger binding thiol ligands, the position of the incorporated QDs can be controlled from centered to off-center and eventually to the surface of the silica spheres. The proposed incorporation mechanism explains how we can have high control over the incorporation of single QDs exactly in the middle of silica spheres. It is likely that the proposed mechanism also applies to the incorporation of other hydrophobic nanocrystals in silica using the same method. In conjunction with our findings, we were able to make QD/silica particles with an unprecedented quantum efficiency of 35%.

We have compared calorimetric measurements with the nonlinear optical technique vibrational sum frequency scattering to investigate interface–solvent effects in colloidal gelation transitions. This allows us to explain the difference in gelation behaviour between dispersions of stearyl-coated silica particles in n-hexadecane and benzene or toluene. In n-hexadecane dispersions, an anomalous heat effect is observed, due to the formation of an ordered interface layer (that is not confined to the first monolayer and is composed of ~1/3 surface crafted chains and ~2/3 solvent molecules). For solvents that cannot interdigitate with the surface chains this transition does not occur and consequently no heat effect is observed.

A method is presented to control the in-plane ordering, size, and interparticle distance of nanoparticles fabricated by evaporation through a mask of colloidal particles. The use of optical tweezers combined with critical point drying gives single-particle position control over the colloidal particles in the mask. This extends the geometry of the colloidal masks from (self-organized) hexagonal to any desired symmetry and spacing. Control over the mask's hole size is achieved by MeV ion irradiation, which causes the colloids to expand in the in-plane direction, thus shrinking the size of the holes. After modification of the mask, evaporation at different angles with respect to the mask gives additional control over structure and interparticle distance, allowing nanoparticles of different materials to be deposited next to each other. We demonstrate large arrays of metal nanoparticles with dimensions in the 15-30 nm range, with control over the interparticle distance and in-plane ordering.

We report on novel possibilities for studying colloidal suspensions in a steady shear field in real space. Fluorescence confocal microscopy is combined with the use of a counter-rotating cone?plate shear cell. This allows imaging of individual particles in the bulk of a sheared suspension in a stationary plane. Moreover, this plane of zero velocity can be moved in the velocity gradient direction while keeping the shear rate constant. The colloidal system under study consists of rhodamine labelled PMMA spheres in a nearly density and refractive index matched mixture of cyclohexylbromide and cis-decalin. We show measured flow profiles in both the fluid and the crystalline phase and find indications for shear banding in the case of a sheared crystal. Furthermore, we show that, thanks to the counter-rotating principle of the cone?plate shear cell, a layer of particles in the bulk of a sheared crystalline suspension can be imaged for a prolonged time, with the result that their positions can be tracked.

A setup is described for simultaneous three-dimensional manipulation and imaging inside a concentrated colloidal dispersion using (time-shared) optical tweezers and confocal microscopy. The use of two microscope objectives, one above and one below the sample, enables imaging to be completely decoupled from trapping. The instrument can be used in different trapping (inverted, upright, and counterpropagating) and imaging modes. Optical tweezers arrays, dynamically changeable and capable of trapping several hundreds of micrometer-sized particles, were created using acousto-optic deflectors. Several schemes are demonstrated to trap three-dimensional colloidal structures with optical tweezers. One combined a Pockels cell and polarizing beam splitters to create two trapping planes at different depths in the sample, in which the optical traps could be manipulated independently. Optical tweezers were used to manipulate collections of particles inside concentrated colloidal dispersions, allowing control over collo...