Automated tracking of colloidal clusters with sub-pixel accuracy and precision

Quantitative tracking of features from video images is a basic technique employed in many areas of science. Here, we present a method for the tracking of features that partially overlap, in order to be able to track so-called colloidal molecules. Our approach implements two improvements into existing particle tracking algorithms. Firstly, we use the history of previously identified feature locations to successfully find their positions in consecutive frames. Secondly, we present a framework for non-linear least-squares fitting to summed radial model functions and analyze the accuracy (bias) and precision (random error) of the method on artificial data. We find that our tracking algorithm correctly identifies overlapping features with an accuracy below 0.2% of the feature radius and a precision of 0.1 to 0.01 pixels for a typical image of a colloidal cluster. Finally, we use our method to extract the three-dimensional diffusion tensor from the Brownian motion of colloidal dimers.Comment: 20 pages, 8 figures. Non-revised preprint version, please refer to http://dx.doi.org/10.1088/1361-648X/29/4/04400

Microparticle assembly pathways on lipid membranes

Understanding interactions between microparticles and lipid membranes is of increasing importance, especially for unraveling the influence of microplastics on our health and environment. Here, we study how a short-ranged adhesive force between microparticles and model lipid membranes causes membrane-mediated particle assembly. Using confocal microscopy, we observe the initial particle attachment to the membrane, then particle wrapping, and in rare cases spontaneous membrane tubulation. In the attached state, we measure that the particle mobility decreases by 26%. If multiple particles adhere to the same vesicle, their initial single-particle state determines their interactions and subsequent assembly pathways: 1) attached particles only aggregate when small adhesive vesicles are present in solution, 2) wrapped particles reversibly attract one another by membrane deformation, and 3) a combination of wrapped and attached particles form membrane-mediated dimers, which further assemble into a variety of complex structures. The experimental observation of distinct assembly pathways induced only by a short ranged membrane-particle adhesion, shows that a cellular cytoskeleton or other active components are not required for microparticle aggregation. We suggest that this membrane-mediated microparticle aggregation is a reason behind reported long retention times of polymer microparticles in organisms.Comment: 20 pages, 11 figures (including supporting material

Diffusion-based height analysis reveals robust microswimmer-wall separation

Microswimmers typically move near walls, which can strongly influence their motion. However, direct experimental measurements of swimmer-wall separation remain elusive to date. Here, we determine this separation for model catalytic microswimmers from the height dependence of the passive component of their mean-squared displacement. We find that swimmers exhibit "ypsotaxis", a tendency to assume a fixed height above the wall for a range of salt concentrations, swimmer surface charges, and swimmer sizes. Our findings indicate that ypsotaxis is activity-induced, posing restrictions on future modeling of their still debated propulsion mechanism

Soft and stiff normal modes in floppy colloidal square lattices

Floppy microscale spring networks are widely studied in theory and simulations, but no well-controlled experimental system currently exists. Here, we show that square lattices consisting of colloid-supported lipid bilayers functionalized with DNA linkers act as microscale floppy spring networks. We extract their normal modes by inverting the particle displacement correlation matrix, showing the emergence of a spectrum of soft modes with low effective stiffness in addition to stiff modes that derive from linker interactions. Evaluation of the softest mode, a uniform shear mode, reveals that shear stiffness decreases with lattice size. Experiments match well with Brownian particle simulations and we develop a theoretical description based on mapping interactions onto linear response to describe the modes. Our results reveal the importance of entropic steric effects, and can be used for developing reconfigurable materials at the colloidal length scale

Thermodynamic equilibrium of binary mixtures on curved surfaces

We study the global influence of curvature on the free energy landscape of two-dimensional binary mixtures confined on closed surfaces. Starting from a generic effective free energy, constructed on the basis of symmetry considerations and conservation laws, we identify several model-independent phenomena, such as a curvature-dependent line tension and local shifts in the binodal concentrations. To shed light on the origin of the phenomenological parameters appearing in the effective free energy, we further construct a lattice-gas model of binary mixtures on non-trivial substrates, based on the curved-space generalization of the two-dimensional Ising model. This allows us to decompose the interaction between the local concentration of the mixture and the substrate curvature into four distinct contributions, as a result of which the phase diagram splits into critical sub-diagrams. The resulting free energy landscape can admit, as stable equilibria, strongly inhomogeneous mixed phases, which we refer to as antimixed states below the critical temperature. We corroborate our semi-analytical findings with phase-field numerical simulations on realistic curved lattices. Despite this work being primarily motivated by recent experimental observations of multi-component lipid vesicles supported by colloidal scaffolds, our results are applicable to any binary mixture confined on closed surfaces of arbitrary geometry.Comment: 20 Pages, 7 Figures; comments and references added, typos correcte

Interface geometry of binary mixtures on curved substrates

Motivated by recent experimental work on multicomponent lipid membranes supported by colloidal scaffolds, we report an exhaustive theoretical investigation of the equilibrium configurations of binary mixtures on curved substrates. Starting from the J\"ulicher-Lipowsky generalization of the Canham-Helfrich free energy to multicomponent membranes, we derive a number of exact relations governing the structure of an interface separating two lipid phases on arbitrarily shaped substrates and its stability. We then restrict our analysis to four classes of surfaces of both applied and conceptual interest: the sphere, axisymmetric surfaces, minimal surfaces and developable surfaces. For each class we investigate how the structure of the geometry and topology of the interface is affected by the shape of the substrate and we make various testable predictions. Our work sheds light on the subtle interaction mechanism between membrane shape and its chemical composition and provides a solid framework for interpreting results from experiments on supported lipid bilayers.Comment: 26 pages, 10 figure

Brownian motion of flexibly-linked colloidal rings

Ring, or cyclic, polymers have unique properties compared to linear polymers, due to their topologically closed structure that has no beginning or end. Experimental measurements on molecular ring polymers are challenging due to their polydispersity in molecular weight and the presence of undesired side products such as chains. Here, we study an experimental model system for cyclic polymers, that consists of rings of flexibly-linked micron-sized colloids with $n$=4..8 segments. We characterize the conformations of these flexible colloidal rings and find that they are freely-jointed up to steric restrictions. We measure their diffusive behavior and compare it to hydrodynamic simulations. Interestingly, flexible colloidal rings have a larger translational and rotational diffusion coefficient compared to colloidal chains. In contrast to chains, their internal deformation mode shows slower fluctuations for $n\lesssim 8$ and saturates for higher values of $n$. We show that constraints stemming from the ring structure cause this decrease in flexibility for small $n$ and infer the expected scaling of the flexibility as function of ring size. Our findings could have implications for the behavior of both synthetic and biological ring polymers, as well as for the dynamic modes of floppy colloidal materials

Power-law intermittency in the gradient-induced self-propulsion of colloidal swimmers

Active colloidal microswimmers serve as archetypical active fluid systems, and as models for biological swimmers. Here, by studying in detail their velocity traces, we find robust power-law intermittency with system-dependent exponential cut off. We model the motion by an interplay of the field gradient-dependent active force and the locally fluctuating hydrodynamic drag, set by the wetting properties of the substrate. The model closely describes the velocity distributions of two disparate swimmer systems: AC field activated and catalytic swimmers. The generality is highlighted by the collapse of all data in a single master curve, suggesting the applicability to further systems, both synthetic and biological.Comment: 5 pages, 3figure