We propose a first-principles model for self-assembled magnetic surface structures on the water-air interface reported in earlier experiments \cite{snezhko2,snezhko4}. The model is based on the Navier-Stokes equation for liquids in shallow water approximation coupled to Newton equations for interacting magnetic particles suspended on the water-air interface. The model reproduces most of the observed phenomenology, including spontaneous formation of magnetic snake-like structures, generation of large-scale vortex flows, complex ferromagnetic-antiferromagnetic ordering of the snake, and self-propulsion of bead-snake hybrids. The model provides valuable insights into self-organization phenomena in a broad range of non-equilibrium magnetic and electrostatic systems with competing interactions.
Bilayer membranes self-assembled from amphiphilic molecules such as lipids, surfactants and block copolymers are ubiquitous in biological and physiochemical systems. The shape and structure of bilayer membranes depend crucially on their mechanical properties such surface tension, bending moduli and line tension. Understanding how the molecular property of the amphiphiles determine the structure and mechanics of the self-assembled bilayers requires a molecularly detailed theoretical framework. The self-consistent field theory provides such a theoretical framework, which is capable of accurately…
We report the experimental discovery of a self-assembled capsule, with density set by interfacial glass beads and an internal bubble, that automatically performs regular oscillations up and down a vial in response to a temperature gradient. Similar composites featuring interfacial particles and multiple internal compartments could be the solution to a variety of application challenges.
We demonstrate that resonant excitation of CdMnTe self-assembled quantum dots creates an ensemble of spin-polarized magnetic polarons at B=0 T. The strong spatial confinement characteristic of quantum dots significantly increases the stability of magnetic polarons so that the optically induced spin alignment is observed for temperatures > 120 K.
We use magnetotunnelling spectroscopy as a non-invasive probe to produce two-dimensional spatial images of the probability density of an electron confined in a self-assembled semiconductor quantum dot. The images reveal clearly the elliptical symmetry of the ground state and the characteristic lobes of the higher energy states.
Using computer simulations, we explore how thermal noise-induced randomness in a self-assembled photonic crystal affects its photonic band gaps (PBGs). We consider a two-dimensional photonic crystal comprised of a self-assembled array of parallel dielectric hard rods of infinite length with circular or square cross section. We find the PBGs can exist over a large range of intermediate packing densities. Counterintuitively, the largest band gap does not always appear at the packing density where the crystal is most ordered, despite the randomness inherent in any self-assembled structure. For ro…
We report many different nano-structures which are formed when model nano-particles of different sizes (diameter σ n ) are allowed to aggregate in a background matrix of semi-flexible self assembled polymeric worm like micellar chains. The different nano-structures are formed by the dynamical arrest of phase-separating mixtures of micellar monomers and nano-particles. The different mor- phologies obtained are the result of an interplay of the available free volume, the elastic energy of deformation of polymers, the density (chemical potential) of the nano-particles in the polymer ma- trix and,…
We outline a strategy for quantitatively evaluating the conformational characteristics of self-assembled structures using the techniques of contrast variation small angle neutron scattering. By means of basis function expansion, a case study of spherical micelles demonstrates that the intra-particle hydration and polymer distributions can be determined from the coherent scattering intensity in a model-free manner. Our proposed approach is simple, analytical and does not require a presumptive hypothesis of scattering function as an input in data analysis. The successful implementation of the pr…
The magnetic field of a cuboidal cluster of eight magnetic spheres is measured. It decays with the inverse seventh power of the distance. This corresponds formally to a hitherto unheard-of multipole, namely a dotriacontapole. This strong decay is explained on the basis of dipole-dipole interaction and the symmetry of the ensuing ground state of the cuboidal cluster. A method to build such dotriacontapoles is provided.
Although buckling is a prime route to achieve functionalization and synthesis of single colloids, buckling of colloidal structures---made up of multiple colloids---remains poorly studied. Here, we investigate the buckling of the simplest form of a colloidal structure, a colloidal chain that is self-assembled through critical Casimir forces. We demonstrate that the mechanical instability of such a chain is strikingly reminiscent of that of classical Euler buckling but with thermal fluctuations and plastic effects playing a significant role. Namely, we find that fluctuations tend to diverge clos…
We study long range density fluctuations (hyperuniformity) in two-dimensional jammed packings of bidisperse droplets. Taking advantage of microfluidics, we systematically span a large range of size and concentration ratios of the two droplet populations. We identify various defects increasing long range density fluctuations mainly due to organization of local particle environment. By choosing an appropriate bidispersity, we fabricate materials with a high level of hyperuniformity. Interesting transparency properties of these optimized materials are established based on numerical simulations.
The transport of motile entities across modulated energy landscapes plays an important role in a range of phenomena in biology, colloidal science and solid-state physics. Here, an easily implementable strategy that allows for the collective and monitored transport of microparticles at fluid-fluid interfaces is introduced. Adsorbed magnetic microparticles are carried on time-dependent magnetic potentials, generated by a dynamic self-assembled lattice of different-sized magnetic particles. In such binary systems, the sudden reorientation of the applied field triggers the rapid exchange between a…
We demonstrate a general method to assemble and propel highly maneuverable colloidal carpets which can be steered via remote control in any direction of the plane. These colloidal micropropellers are composed by an ensemble of spinning rotors and can be readily used to entrap, transport, and release biological cargos on command via a hydrodynamic conveyor-belt effect. An efficient control of the cargo transportation combined with remarkable "healing" ability to surpass obstacles demonstrate a great potential towards development of multifunctional smart devices at the microscale.
Ice-templating, also referred to as freeze-casting, is a process exploiting unidirectional crystallization of ice to structure macroporous materials from colloidal solutions. Commonly applied to inorganic and polymeric materials, we employ it here to cast soft self-assembled matter into spongy solid foams. Use of ice-templating to cast soft matter is generally confined to polymers. In the case of polymeric hydrogels, cross-linking ensures a good stability towards the harsh conditions (fast cooling at temperatures as low as-80{\textdegree}C) employed during ice-templating. However, freeze-casti…
We investigate the length distribution of self-assembled, long and stiff polymers at thermal equilibrium. Our analysis is based on calculating the partition functions of stiff polymers of variable lengths in the elastic regime. Our conclusion is that the length distribution of this self-assembled system follows closely the exponential distribution, except at the short length limit. We then discuss the implications of our results on the experimentally observed length distributions in amyloid fibrils.
We show that the stacking of flat aromatic molecules on a curved surface results in topological defects. We consider, as an example, spherical vesicles, self-assembled from molecules with 5- and 6-thiophene cores. We predict that the symmetry of the molecules influences the number of topological defects and the resulting equilibrium shape.
Patterns generated by a colloidal suspension of nanospheres drying on a frictional substrate are studied by experiments and computer simulations. The obtained two-dimensional self-assembled structures are commonly used for nanosphere lithography. A spring-block stick-slip model is introduced for simulating the phenomenon and the influence of several controllable parameters on the final structure is investigated. The model successfully reproduces the experimentally observed patterns and the dynamics leading to pattern formation is revealed.
In this article, a dynamical force microscopy study of self-assembled monolayers of organosilanes, grafted on a silica support, is reported. Organosilanes, terminated either with a functional group (ethylene glycol) or with a methyl group, were used. The influence of the reaction time and the solvent composition on the grafting was investigated to improve the homogeneity of the self-assembled monolayers. Numerical simulations of approach-retract curves, obtained in the tapping mode, were performed and compared to experimental ones. Informations, such as mechanical response and height of the gr…
The criticality of self-assembled rigid rods on triangular lattices is investigated using Monte Carlo simulation. We find a continuous transition between an ordered phase, where the rods are oriented along one of the three (equivalent) lattice directions, and a disordered one. We conclude that equilibrium polydispersity of the rod lengths does not affect the critical behavior, as we found that the criticality is the same as that of monodisperse rods on the same lattice, in contrast with the results of recently published work on similar models.
A critical step in tissue engineering is the design and synthesis of 3D biocompatible matrices (scaffolds) to support and guide the proliferation of cells and tissue growth. Most existing techniques rely on the processing of scaffolds under controlled conditions and then implanting them \textit{in vivo}, with questions related to biocompatibility and the implantation process that are still challenging. As an alternative, it was proposed to assemble the scaffolds \textit{in loco} through the self-organization of colloidal particles mediated by cells. In this study, we combine experiments, parti…
Physics governing the locomotion of microorganisms and other microsystems is dominated by viscous damping. An effective swimming strategy involves the non-reciprocal and periodic deformations of the considered body. Here, we show that a magnetocapillary-driven self-assembly, composed of three soft ferromagnetic beads, is able to swim along a liquid-air interface when powered by an external magnetic field. More importantly, we demonstrate that trajectories can be fully controlled, opening ways to explore low Reynolds number swimming. This magnetocapillary system spontaneously forms by self-asse…
The dynamics of phase separation in multi-component bilayer fluid vesicles is investigated by means of large-scale dissipative particle dynamics. The model explicitly accounts for solvent particles, thereby allowing for the very first numerical investigation of the effects of hydrodynamics and area-to-volume constraints. We observed regimes corresponding to coalescence of flat patches, budding and vesiculation, and coalescence of caps. We point out that the area-to-volume constraint has a strong influence on crossovers between these regimes.
The elastic properties of a self-assembled bilayer membrane are studied using the self-consistent field theory, applied to a model system composed of flexible amphiphilic chains dissolved in hydrophilic polymeric solvents. Examining the free energy of bilayer membranes with different geometries allows us to calculate their bending modulus, Gaussian modulus, two fourth-order membrane moduli, and the line tension. The dependence of these parameters on the microscopic characteristics of the amphiphilic chain, characterized by the volume fraction of the hydrophilic component, is systematically stu…
Colloidal inclusions in lab-on-a-chip devices can be used to perform analytic operations in a non-invasive fashion. We demonstrate here a novel approach to realize fast and reversible micro-sieving operations by manipulating and transporting colloidal chains via mobile domain walls in a magnetic structured substrate. We show that this technique allows to precisely move and sieve non-magnetic particles, to tweeze microscopic cargos or to mechanically compress highly dense colloidal monolayers.
A systematic investigation of the phase separation dynamics in self-assembled multi-component bilayer fluid vesicles and open membranes is presented. We use large-scale dissipative particle dynamics to explicitly account for solvent, thereby allowing for numerical investigation of the effects of hydrodynamics and area-to-volume constraints. In the case of asymmetric lipid composition, we observed regimes corresponding to coalescence of flat patches, budding, vesiculation and coalescence of caps. The area-to-volume constraint and hydrodynamics have a strong influence on these regimes and the cr…
A technique to measure microscopic rotational motion is presented. When a small fluorescent polystyrene microsphere is attached to a larger polystyrene microsphere, the larger sphere acts as a lens for the smaller microsphere and provides an optical signal that is a strong function of the azimuthal angle. We demonstrate the technique by measuring the rotational diffusion constant of the microsphere in solutions of varying viscosity and discuss the feasibility of using this probe to measure rotational motion of biological systems.
We present results from particle simulations with isotropic medium range interactions in two dimensions. At low temperature novel types of aggregated structures appear. We show that these structures can be explained by spontaneous symmetry breaking in analytic solutions to an adaptation of the spherical spin model. We predict the critical particle number where the symmetry breaking occurs and show that the resulting phase diagram agrees well with results from particle simulations.
We analyze transmission electron microscopy (TEM) images of self-assembled quasicrystals, composed of binary systems of nanoparticles. We use an automated procedure that identifies the positions of dislocations and determines their topological character. To achieve this we decompose the quasicrystal into its individual density modes, or Fourier components, and identify their topological winding numbers for every dislocation. This procedure associates a Burgers function with each dislocation, from which we extract the components of the Burgers vector after choosing a basis. The Burgers vectors …
We investigate the nature of the ordered phase and the orientational correlations between adjacent layers of the confined three-dimensional self-assembled rigid rod model, on the cubic lattice. We find that the ordered phase at finite temperatures becomes uniaxial in the thermodynamic limit, by contrast to the ground state (partial) order where the orientation of the uncorrelated layers is perpendicular to one of the three lattice directions. The increase of the orientational correlation between layers as the number of layers increases suggests that the unconfined model may also exhibit uniaxi…
