Publications by authors named "Dullens R"

The curvature of elongated microscopic building blocks plays a crucial role on their self-assembly into orientationally ordered phases. While rod-like molecules form a handful of liquid crystal (LC) phases, curved or banana-shaped molecules show more than fifty phases, with fascinating physical properties, such as chirality or polarity. Despite the fundamental and technological importance of these so-called 'banana-shaped liquid crystals', little is known about their microscopic details at the single-molecule level.

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Colloid science has recently grown substantially owing to the innovative use of silane coupling agents (SCAs), especially 3-trimethoxysilylpropyl methacrylate (TPM). SCAs were previously used mainly as modifying agents, but their ability to form droplets and condense onto pre-existing structures has enabled their use as a versatile and powerful tool to create novel anisotropic colloids with increasing complexity. In this Review, we highlight the advances in complex colloid synthesis facilitated by the use of TPM and show how this has driven remarkable new applications.

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We present a technique for measuring the interactions between pairs of colloidal particles in two optical traps. This method is particularly suitable for measuring strongly attractive potentials, an otherwise challenging task. The interaction energy is calculated from the distribution of inter-particle separations by accounting for the contribution from the optical traps with arbitrary trap profiles.

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During devitrification, pre-existing crystallites grow by adding particles to their surface via a process that is either thermally activated (diffusive mode) or happens without kinetic barriers (fast crystal growth mode). It is yet unclear what factors determine the crystal growth mode and how to predict it. With simulations of repulsive hard-sphere-like (Weeks-Chandler-Andersen) glasses, we show for the first time that the same system at the same volume fraction and temperature can devitrify via both modes depending on the preparation protocol of the glass.

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We perform feedback experiments and simulations in which a colloidal dumbbell particle, acting as a particle on a ring, is followed by a repulsive optical trap controlled by a continuous-time-delayed feedback protocol. The dynamics are described by a persistent random walk similarly to that of an active Brownian particle, with a transition from predominantly diffusive to driven behavior at a critical delay time. We model the dynamics in the short and long delay regimes using stochastic delay differential equations and derive a condition for stable driven motion.

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Anisotropic colloidal particles exhibit complex dynamics which play a crucial role in their functionality, transport, and phase behavior. In this Letter, we investigate the two-dimensional diffusion of smoothly curved colloidal rods-also known as colloidal bananas-as a function of their opening angle α. We measure the translational and rotational diffusion coefficients of the particles with opening angles ranging from 0^{∘} (straight rods) to nearly 360^{∘}(closed rings).

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We optimize and characterize the preparation of 3-trimethoxysilyl propyl methacrylate (TPM) colloidal suspensions for three-dimensional confocal microscopy. We revisit a simple synthesis of TPM microspheres by nucleation of droplets from prehydrolyzed TPM oil in a "zero-flow" regime and demonstrate how precise and reproducible control of particle size may be achieved via single-step nucleation with a focus on how the reagents are mixed. We also revamp the conventional dyeing method for TPM particles to achieve uniform transfer of a fluorophore to the organosilica droplets, improving particle identification.

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We study the crystallization of colloidal dispersions under capillary-action-induced shear as the dispersion is drawn into flat walled capillaries. Using confocal microscopy and small angle x-ray scattering, we find that the shear near the capillary walls influences the crystallization to result in large random hexagonal close-packed (RHCP) crystals with long-range orientational order over tens of thousands of colloidal particles. We investigate the crystallization mechanism and find partial crystallization under shear, initiating with hexagonal planes at the capillary walls, where shear is highest, followed by epitaxial crystal growth from these hexagonal layers after the shear is stopped.

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Unlike crystals, glasses age or devitrify over time, reflecting their nonequilibrium nature. This lack of stability is a serious issue in many industrial applications. Here, we show by numerical simulations that the devitrification of quasi-hard-sphere glasses is prevented by suppressing volume-fraction inhomogeneities.

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Article Synopsis
  • Scientists are studying how tiny particles, like colloidal bananas, can come together to form complicated shapes and structures all by themselves.
  • They discovered a new structure called the vortex phase, which forms because of the way these banana-shaped particles fit together and move around each other.
  • This research shows that these amazing shapes can form just because of the different sizes and shapes of the particles, without needing any special tools or forces!
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Surface roughness plays an important role in determining the mechanical properties, wettability, and self-assembly in colloidal systems. In this work, we develop a simple and fast method to produce rough colloidal SU-8 rods, bananas, and spheres, via the nanoprecipitation of SU-8 in water. During this process, SU-8 nanospheres are absorbed onto the surface of the colloidal SU-8 particles and then cross-linked using UV-light.

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Photo-catalytically active crystalline TiO2 has attracted special attention due to its relevance for renewable energy and is typically obtained by the calcination of amorphous TiO2. However, stabilising hollow colloidal TiO2 particles against aggregation during calcination without compromising their photocatalytic activity poses two conflicting demands: to be stable their surface needs to be coated, while efficient photocatalysis requires an exposed TiO2 surface. Here, this incompatibility is resolved by partially coating TiO2 shells with evenly distributed 3-trimethoxysilyl propyl methacrylate (TPM) lobes.

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Understanding the impact of curvature on the self-assembly of elongated microscopic building blocks, such as molecules and proteins, is key to engineering functional materials with predesigned structure. We develop model "banana-shaped" colloidal particles with tunable dimensions and curvature, whose structure and dynamics are accessible at the particle level. By heating initially straight rods made of SU-8 photoresist, we induce a controllable shape deformation that causes the rods to buckle into banana-shaped particles.

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The effect of hydrodynamic interactions (HI) on the long-time self-diffusion in quasi-two-dimensional fluids of paramagnetic colloidal particles is investigated using a combination of experiments and Brownian dynamics (BD) simulations. In the BD simulations, the direct interactions (DI) between the particles consist of a short-ranged repulsive part and a long-ranged part that is proportional to 1/r^{3}, with r the interparticle distance. By studying the equation of state, the simulations allow for the identification of the regime where the properties of the fluid are fully controlled by the long-ranged interactions, and the thermodynamic state solely depends on the dimensionless interaction strength Γ.

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The properties of a wide range of two-dimensional network materials are investigated by developing a generalized network theory. The methods developed are shown to be applicable to a wide range of systems generated from both computation and experiment; incorporating atomistic materials, foams, fullerenes, colloidal monolayers, and geopolitical regions. The ring structure in physical networks is described in terms of the node degree distribution and the assortativity.

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We report a straightforward, model-free approach for measuring pair potentials from particle-coordinate data, based on enforcing consistency between the pair distribution function measured separately by the distance-histogram and test-particle insertion routes. We demonstrate the method's accuracy and versatility in simulations of simple fluids, before applying it to an experimental system composed of superparamagnetic colloidal particles. The method will enable experimental investigations into many-body interactions and allow for effective coarse graining of interactions from simulations.

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We describe the synthesis and application of 3-(trimethoxysilyl)propyl methacrylate (TPM) particles as a colloidal model system for three-dimensional (3D) confocal scanning laser microscopy. The effect of the initial TPM concentration on the growth and polydispersity of the particles and a recently developed solvent transfer method to disperse particles in a refractive index and density-matching solvent mixture are reviewed and discussed. To fully characterize the system as a colloidal model, we measure the pair potential between the TPM particles directly using optical tweezers.

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The bulk synthesis of fluorescent colloidal SU-8 polymer rods with tunable dimensions is described. The colloidal SU-8 rods are prepared by shearing an emulsion of SU-8 polymer droplets and then exposing the resulting non-Brownian rods to ultrasonic waves, which breaks them into colloidal rods with typical lengths of 3.5-10 µm and diameters of 0.

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Colloidal particles with asymmetric catalytic activities are emerging micro/nanomotors that harvest chemical energy for propulsion in fluids. It is of general interest to produce such particles with high performance, in large quantity and at low cost. In this paper, we present a facile bulk method to synthesize silver-head colloidal silica rods.

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The formation and kinetics of grain boundaries are closely related to the topological constraints imposed on their complex dislocation structure. Loop-shaped grain boundaries are unique structures to establish such a link because their overall topological "charge" is zero due to their null net Burgers vector. Here, we observe that a local rotational deformation of a 2D colloidal crystal with an optical vortex results in a grain boundary loop only if the product of its radius and misorientation exceeds a critical value.

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Recent progress in synthetic nanotechnology and the ancient use of metals in food preservation and the antibacterial treatment of wounds have prompted the development of nanometallic materials for antimicrobial applications. However, the materials designed so far do not simultaneously display antimicrobial activity and the capability of binding and capturing bacteria and spores. Here, we develop a one-step pyrolysis procedure to synthesize monodisperse superparamagnetic nickel colloidal nanocrystal clusters (SNCNCs), which show both antibacterial activity and the ability to bind Gram-positive (Bacillus subtilis) and Gram-negative (Escherichia coli) bacteria, as well as bacterial spores.

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Article Synopsis
  • Scientists used a special theory, called DDFT, to study how small hard disks (like balls) move and relax when packed closely together.
  • They looked at both theoretical results and real-life experiments and found they matched well when the disks weren't too tightly packed.
  • However, when the disks were packed really tight, the experiments showed different results from the theory, especially because the liquids around them had strong effects on how they moved.
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Recently, the full phase behaviour of 2D colloidal hard spheres was experimentally established, and found to involve a first order liquid to hexatic transition and a continuous hexatic to crystal transition (Thorneywork et al 2017 Phys. Rev. Lett.

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Confocal microscopy was used to directly observe the structural coarsening of the first layer of short colloidal rods sedimented onto a flat wall. Based on an image analysis algorithm we devised, quantitative information on the location, orientation and length of each particle can be extracted with high precision. At high density the system undergoes structural arrest, and becomes trapped in a disordered state of randomly arranged filaments that are composed of side-by-side aligned rods.

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