Nanoparticles with "sticky patches" have long been proposed as building blocks for the self-assembly of complex structures. The synthetic realizability of such patchy particles, however, greatly lags behind predictions of patterns they could form. Using computer simulations, we show that structures of the same genre can be obtained from a solution of simple isotropic spheres, provided control only over their sizes and a small number of binding affinities. In a first step, finite clusters of well-defined structure and composition emerge from natural dynamics with high yield. In effect a kind of patchy particle, these clusters can further assemble into a variety of complex superstructures, including filamentous networks, ordered sheets, and highly porous crystals.
We present a generic model to describe the fractal self-assembly of proteins in terms of electrostatic and hydrophobic interactions. The predictions of the model were correlated with the simulated fractals obtained using patchy diffusion-limited aggregation, and the experimentally observed Amyloid-\b{eta} (A\b{eta}) fractal self-assembly using confocal microscopy. The molecular docking was used to determine the properties of the patches on A\b{eta} oligomers. Similar patch properties were used to design the particles for simulation. In agreement with the model predictions, the free energy of f…
Intimately connected to the rule of life, chirality remains a long-time fascination in biology, chemistry, physics and materials science. Chiral structures, e.g., nucleic acid and cholesteric phase developed from chiral molecules are common in nature and synthetic soft materials. While it was recently discovered that achiral but bent core mesogens can also form chiral helices, the assembly of chiral microstructures from achiral polymers has rarely been explored. Here, we reveal chiral emergence from achiral conjugated polymers for the first time, in which hierarchical helical structures are de…
We propose a general framework for solving inverse self-assembly problems, i.e. designing interactions between elementary units such that they assemble spontaneously into a predetermined structure. Our approach uses patchy particles as building blocks, where the different units bind at specific interaction sites (the patches), and we exploit the possibility of having mixtures with several components. The interaction rules between the patches is determined by transforming the combinatorial problem into a Boolean satisfiability problem (SAT) which searches for solutions where all bonds are forme…
Patchy particles have received great attention due to their ability to develop directional and selective interactions and serve as building units for the self-assembly of innovative colloidal molecules and crystalline structures. Although synthesizing particles with multiple dissimilar patches is still highly challenging and lacks efficient methods, these building blocks would open paths towards a broader range of ordered materials with inherent properties. Herein, we describe a new approach to pattern functional DNA patches at the surface of particles, by the use of colloidal stamps. DNA inks…
Manipulating the way in which colloidal particles self-organise is a central challenge in the design of functional soft materials. Meeting this challenge requires the use of building blocks that interact with one another in a highly specific manner. Their fabrication, however, is limited by the complexity of the available synthesis procedures. Here, we demonstrate that, starting from experimentally available magnetic colloids, we can create a variety of complex building blocks suitable for hierarchical self-organisation using a simple scalable process. Using computer simulations, we compress s…
Just like atoms combine into molecules, colloids can self-organize into predetermined structures according to a set of design principles. Controlling valence -- the number of inter-particle bonds -- is a prerequisite for the assembly of complex architectures. The assembly can be directed via solid `patchy' particles with prescribed geometries to make, for example, a colloidal diamond. We demonstrate here that the nanoscale ordering of individual molecular linkers can combine to program the structure of microscopic assemblies. Specifically, we experimentally show that covering initially isotrop…
Colloidal molecules are designed to mimic their molecular analogues through their anisotropic shape and interactions. However, current experimental realizations are missing the structural flexibility present in real molecules thereby restricting their use as model systems. We overcome this limitation by assembling reconfigurable colloidal molecules from silica particles functionalized with mobile DNA linkers in high yields. We achieve this by steering the self-assembly pathway towards the formation of finite-sized clusters by employing high number ratios of particles functionalized with comple…
Creating materials with structure that is independently controllable at a range of scales requires breaking naturally occurring hierarchies. Breaking these hierarchies can be achieved via the decoupling of building block attributes from structure during assembly. Here, we demonstrate both geometric and interaction decoupling in pre-assembled colloidal structures of cube-like particles with rounded edges. Through computer simulations and experiments, we show that compressing a small number of such cubes in spherical confinement results in clusters with highly reproducible structures that can be…
Brownian Dynamics is used to study self-assembly in a hybrid system of istotropic particles (IPs), combined with anisotropic building blocks that represent special "designer particles". Those are modeled as spherical patchy particles (PPs) with binding only allowed between their patches and IPs. In this study, two types of PPs are considered: Octahedral PPs (Oh-PPs) and Square PPs (Sq-PPs), with octahedral and square arrangements of patches, respectively. The self-assembly is additionally facilitated by the simulated annealing procedure. The resultant structures are characterized by a combinat…
Self-organized complex structures in nature, e.g. viral capsids, hierarchical biopolymers, and bacterial flagella, offer efficiency, adaptability, robustness, and multi-functionality. Can we program the self-assembly of three-dimensional (3D) complex structures with simple building blocks, and reach similar or higher level of sophistication in engineered materials? Here we present an analytic theory of tetrahedral nanoparticles (NPs) self-assembling in 3D space, where unavoidable geometrical frustration combined with competing attractive and repulsive inter-particle interactions lead to contro…
Shape-dependent oriented trapping and scaffolding of plasmonic nanoparticles by topological defects for self-assembly of colloidal dimers in liquid crystals
