The growing interest in the non-equilibrium assembly of colloidal particles in active liquids is driven by the motivation to create novel structures endowed with tunable properties unattainable within the confines of equilibrium systems. Here, we present an experimental investigation of the structural features of colloidal assemblies in active liquids of chiral E. coli. The colloidal particles form dynamic clusters due to the effective interaction mediated by active media. The activity and chirality of the swimmers strongly influence the dynamics and local ordering of colloidal particles, resulting in clusters with persistent rotation, whose structure differs significantly from those in equilibrium systems with attractive interactions, such as colloid-polymer mixtures. The colloid-bacteria mixture displays several hallmark features of a percolation transition at a critical density, where the clusters span the system size. However, a closer examination of the critical exponents associated with cluster size distribution, average cluster size, and correlation length in the vicinity of the critical density suggest strong deviations from the prediction of the standard continuum percolation model. Therefore, our experiments reveal a richer phase behavior of colloidal assemblies in active liquids.
Patchy colloidal platelets with convex, non-spherical shapes have been realized with different materials at length scales ranging from nanometers to microns. While the assembly of these hard shapes tends to maximize edge-to-edge contacts, as soon as a directional attraction is added -- by means of, e.g., specific ligands along the particle edges -- a competition between shape and bonding anisotropy sets in, giving rise to a complex assembly scenario. We focus here on a two-dimensional system of patchy rhombi, i.e., colloidal platelets with a regular rhombic shape decorated with bonding sites a…
Disordered dielectrics with structural correlations on length scales comparable to visible light wavelengths exhibit complex optical properties. Such materials exist in nature, leading to beautiful structural non-iridescent color, and they are also increasingly used as building blocks for optical materials and coatings. In this article, we study the single-scattering properties of micron-sized, disordered colloidal assemblies. The aggregates act as structurally colored supraparticles or as building blocks for macroscopic photonic glasses. We present experimental data for the differential scatt…
The postulate of the existence of a jamming phase diagram (Liu and Nagel, Nature 396, 21 EP (1998aa)) provides a theoretical basis for the classification of a wide range of amorphous solids (colloidal, molecular and emulsion glasses, colloidal and polymer gels, foams and granular matter) on the basis of whether these materials are in the jammed or unjammed state. Whilst such simple classification is appealing, it fails to capture that the criterion of rigidity of such amorphous solids may be defined with respect to a particular deformation orientation or mode (i.e. shear, extrusion, consolidat…
Application of Machine Learning for the Identification of 2D Colloidal Assemblies: A Case Study on Particles of Distinct Shapes
Astrakhan Tatishchev State University（阿斯特拉罕塔季谢夫国立大学）；Caspian Institute of Maritime and River Transport named after Admiral General F.M. Apraksin – the affiliation of “Volga State University of Water Transport”（以海军上将F.M.阿普拉克辛命名的里海海事和河运学院——伏尔加水运大学下属机构）
Rigidity percolation (RP) occurs when mechanical stability emerges in disordered networks as constraints or components are added. Here we discuss RP with structural correlations, an effect ignored in classical theories albeit relevant to many liquid-to-amorphous-solid transitions, such as colloidal gelation, which are due to attractive interactions and aggregation. Using a lattice model, we show that structural correlations shift RP to lower volume fractions. Through molecular dynamics simulations, we show that increasing attraction in colloidal gelation increases structural correlation and th…
We combine experiments, theory, and simulations to investigate the coexistence of nonequilibrium phases emerging from interacting colloidal particles that are electrokinetically propelled in a nematic liquid crystal solvent. We directly determine the mechanical pressure within the radial assemblies and measure a non-equilibrium equation of state for this athermal driven system. A generic model combines phoretic propulsion with the interplay between electrostatic effects and liquid-crystal-mediated hydrodynamics, which are effectively cast into a long-range interparticle repulsion, while elasti…
Biological cells self-organize into living materials that uniquely blend structure with functionality and responsiveness to the environment. The integration of similar life-like features in man-made materials remains challenging, yet desirable to manufacture active, adaptive and autonomous systems. Here we show the self-organization of programmable random lasers from the reversible out-of-equilibrium self-assembly of colloids. Random lasing originates from the optical amplification of light undergoing multiple scattering within the dissipative colloidal assemblies and therefore is crucially de…
Insight in the structure of nanoparticle assemblies up to a single particle level is key to understand the collective properties of these assemblies, which critically depend on the individual particle positions and orientations. However, the characterization of large, micron sized assemblies containing small, 10-500 nanometer, sized colloids is highly challenging and cannot easily be done with the conventional light, electron or X-ray microscopy techniques. Here, we demonstrate that focused ion beam-scanning electron microscopy (FIB-SEM) tomography in combination with image processing enables …
The design of complex materials and the formation of specific patterns often arise from the properties of the individual building blocks. In this respect, colloidal systems offer a unique opportunity because nowadays they can be synthesized in the laboratory with many different shapes and features. Hence, an appropriate choice of the particle characteristics makes it possible to generate macroscopic structures with desired properties. The versatility of colloids can also be explored in two dimensions, using liquid-liquid or air-liquid interfaces as privileged substrates where they can adsorb a…
Melanin is a ubiquitous natural pigment that exhibits broadband absorption and high refractive index. Despite its widespread use in structural color production, how the absorbing material, melanin, affects the generated color is unknown. Using a combined molecular dynamics and finite-difference time-domain computational approach, this paper investigates structural color generation in one-component melanin nanoparticle-based supra-assemblies (called supraballs) as well as binary mixtures of melanin and silica (non-absorbing) nanoparticle-based supraballs. Experimentally produced one-component m…
A fresh approach to the data from experiments with hard sphere colloids yields seminal insights into the glass transition. The precise determination of the fraction of particles caged by their neighbours is unprecedented and provides cornerstone of our study. We show that the so-called "dramatic slowing" that accompanies super-packing is due to correlated cage fluctuations, rather than caging per se. Their statistics establish that the amorphous assemblies of caged particles are in states of self-organised criticality. The implied connection between the onset of caging and the thermodynamic 1s…
Using video microscopy, we measure local spatial constraints in disordered binary colloidal samples, ranging from dilute fluids to jammed glasses, and probe their spatial and temporal correlations to local dynamics during the glass transition. We observe the emergence of significant correlations between constraints and local dynamics within the Lindemann criterion, which coincides with the onset of glassy dynamics in supercooled liquids. Rigid domains in fluids are identified based on local constraints, and demonstrate a percolation transition near glass transition, accompanied by the emergenc…
The propagation of chirality across scales is a common but poorly understood phenomenon in soft matter. In this work, we use computer simulations to study chiral monolayer assemblies formed by hard rod-like colloidal particles in the presence of non-adsorbing polymer and characterize the thermodynamic driving forces responsible for the twisting. Simulations show that straight (achiral) rods assemble into monolayers with a spontaneous twist that is either left- or right-handed, while helical (chiral) rods lead to assemblies with preferential chiral features that depend on their handedness and c…
Phase Behavior and Selectivity of DNA-linked Nanoparticle Assemblies
我们提出了一个模型，可以解释实验观察到的DNA-纳米粒子组装体的相行为（R。Jin等人，JACS 125，1643（2003）; T. A. Taton等人，Science 289，1757（2000））。溶解的DNA连接体与DNA包覆的纳米颗粒的结合可以通过利用服从分数统计的量子颗粒的类比来描述。根据实验结果，我们预测的纳米胶体的相分离温度增加的DNA覆盖的胶体表面。加入盐后，分层温度随盐浓度的增加而增加。我们的分析提出了一种实验策略，将微观DNA序列映射到DNA纳米颗粒溶液的宏观相行为上。这种方法应该提高检测特定DNA序列中（单个）突变的方法的效率。
In many physical and biological systems, particles and microorganisms move in the proximity of an interface. Understanding the dynamics of a particle suspended close to an interface is not only important conceptually but is crucial for practical applications ranging from the treatment of waste waters to industrial applications of self-assemblies. In this work, we experimentally investigate the effects of colloidal weight on its dynamics while moving in the close proximity of a variety of liquid-solid and liquid-air interfaces. Using an upward magnetic force, we change the effective weight of a…
The dynamical arrest of attractive colloidal particles into out-of-equilibrium structures, known as gelation, is central to biophysics, materials science, nanotechnology, and food and cosmetic applications, but a complete understanding is lacking. In particular, for intermediate particle density and attraction, the structure formation process remains unclear. Here, we show that the gelation of short-range attractive particles is governed by a nonequilibrium percolation process. We combine experiments on critical Casimir colloidal suspensions, numerical simulations, and analytical modeling with…
To gain insight into the kinetics of colloidal gel evolution at low particle volume fractions $ϕ$, we utilize differential dynamic microscopy to investigate particle aggregation, geometric percolation, and the subsequent transition to nonergodic dynamics. We report the emergence of unexpectedly rich multiscale dynamics upon the onset of nonergodicity, which separates the wave vectors $q$ into three different regimes. In the high-$q$ domain, the gel exhibits $ϕ$-independent internal vibrations of fractal clusters. The intermediate-$q$ domain is dominated by density fluctuations at the length sc…
Colloidal particles at complex fluid interfaces and within films assemble to form ordered structures with high degrees of symmetry via interactions that include capillarity, elasticity, and other fields like electrostatic charge. Here we study microparticle interactions within free-standing smectic-A films, in which the elasticity arising from the director field distortion and capillary interactions arising from interface deformation compete to direct the assembly of motile particles. New colloidal assemblies and patterns, ranging from 1D chains to 2D aggregates, sensitive to the initial wetti…
The aggregation of attractive colloids has been extensively studied from both theoretical and experimental perspectives as the fraction of solid particles is changed, and the range, type and strength of attractive or repulsive forces between particles varies. The resulting gels consisting of disordered assemblies of attractive colloidal particles, have also been investigated with regards to percolation, phase separation, and the mechanical characteristics of the resulting fractal networks. Despite tremendous progress in our understanding of the gelation process, and the exploration of differen…
Rigidity percolation (RP) is the emergence of mechanical stability in networks. Motivated by the experimentally observed fractal nature of materials like colloidal gels and disordered fiber networks, we study RP in a fractal network. Specifically, we calculate the critical packing fractions of site-diluted lattices of Sierpiński gaskets (SG's) with varying degrees of fractal iteration. Our results suggest that although the correlation length exponent and fractal dimension of the RP of these lattices are identical to that of the regular triangular lattice, the critical volume fraction is dramat…
We study the self-assembly of branching-chain networks and crystals in a binary colloidal system with tunable interactions. The particle positions are extracted from microscope images and order parameters are extracted by image processing and statistical analysis. With these, we construct phase diagrams with respect to particle density, ratio and interaction. In order to draw a more complete picture, we complement the experiments with computer simulations. We establish a region in the phase diagram, where bead ratios and interactions are symmetric, promoting percolated structures.
Equilibrium gels of colloidal particles can be realized through the introduction of a second species, a linker that mediates the bonds between the colloids. A gel forming binary mixture whose linkers can self-assemble into linear chains while still promoting the aggregation of particles is considered in this work. The particles are patchy particles with $f_C$ patches of type $C$ and the linkers are patchy particles with $2$ patches of type $A$ and $f_B$ patches of type B. The bonds between patches of type $A$ ($AA$ bonds) promote the formation of linear chains of linkers. Two different ways (m…
