Chirality frustrates and shapes the assembly of flexible filaments in rope-like, twisted bundles and fibers by introducing gradients of both filament shape (i.e. curvature) and packing throughout the structure. Previous models of chiral filament bundle formation have shown that this frustration gives rise to several distinct morphological responses, including self-limiting bundle widths, anisotropic domain (tape-like) formation and topological defects in the lateral inter-filament order. In this paper, we employ a combination of continuum elasticity theory and discrete filament bundle simulations to explore how these distinct morphological responses compete in the broader phase diagram of chiral filament assembly. We show that the most generic model of bundle formation exhibits at least four classes of equilibrium structure -- finite-width, twisted bundles with isotropic and anisotropic shapes, with and without topological defects, as well as bulk phases of untwisted, columnar assembly (i.e. "frustration escape"). These competing equilibrium morphologies are selected by only a relatively small number of parameters describing filament assembly: bundle surface energy, preferred chiral twist and stiffness of chiral filament interactions, and mechanical stiffness of filaments and their lateral interactions. Discrete filament bundle simulations test and verify continuum theory predictions for dependence of bundle structure (shape, size and packing defects of 2D cross section) on these key parameters.
Bundles of filaments are subject to geometric frustration: certain deformations (e.g. bending while twisted) require longitudinal variations in spacing between filaments. While bundles are common -- from protein fibers to yarns -- the mechanical consequences of longitudinal frustration are unknown. We derive a geometrically-nonlinear formalism for bundle mechanics, using a gauge-like symmetry under reptations along filament backbones. We relate force balance to orientational geometry and assess the elastic cost of frustration in twisted toroidal bundles.
We investigate the equilibrium morphologies of linear and ring-shaped magnetic filaments made from crosslinked ferromagnetic spherical or ellipsoidal colloidal particles. Using Langevin dynamics simulations, we calculate the radius of gyration and total magnetic moment of a single filament at zero field and different temperatures, analyzing the influence of the particles shape, the strength of their magnetic moment and the filament length. Our results show that, among such parameters, the shape of the particles has the strongest qualitative impact on the equilibrium behavior of the filaments.
We investigate with experiments and novel mapping the structure of a hexagonally ordered filament bundle that is held near its ends and progressively twisted around its central axis. The filaments are free to slide relative to each other and are further held under tension-free boundary conditions. Measuring the bundle packing with micro x-ray imaging, we find that the filaments develop the helical rotation $Ω$ imposed at the boundaries. We then show that the observed structure is consistent with a mapping of the filament positions to disks packed on a dual non-Euclidean surface with a Gaussian…
We study the equilibrium morphologies of a single supramolecular magnetic filament in a three-dimensional system as a function of the effective strength of the magnetic dipolar interactions. The study is performed by means of Langevin dynamics simulations with a bead-spring chain model of freely rotating dipoles. We demonstrate the existence of three structural regimes as the value of the dipolar coupling parameter is increased: a coil compaction regime, a coil expansion regime and a closed chain regime in which the structures tend progressively to an ideal ring configuration. We discuss the g…
Densely-packed bundles of biological filaments (filamentous proteins) are common and critical structural elements in range of biological materials. While most bundles form from intrinsically straight filaments, there are notable examples of protein filaments possessing a natural, or intrinsic, curvature, such as the helical bacterial flagellum. We study the non-linear interplay between thermodynamic preference for dense and regular inter-filament packing and the mechanical preference for uniform filament shape in bundles of helically-curved filaments. Geometric constraints in bundles make perf…
Cohesive assemblies of filaments are a common structural motif found in diverse contexts, ranging from biological materials such as fibrous proteins, to artificial materials such as carbon nanotube ropes and micropatterned filament arrays. In this paper, we analyze the complex dependence of cohesive energy on twist, a key structural parameter of both self-assembled and fabricated filament bundles. Based on the analysis of simulated ground states of cohesive bundles, we show that the non-linear influence of twist derives from two distinct geometric features of twisted bundles: (i) the geometric…
Geometric frustration arises whenever the constituents of a physical assembly locally favor an arrangement that cannot be realized globally. Recently, such frustrated assemblies were shown to exhibit filamentation, size limitation, large morphological variations and other exotic response properties. While these unique characteristics can be shown to be a direct outcome of the geometric frustration, some geometrically frustrated systems do not exhibit any of the above phenomena. In this work we exploit the intrinsic approach to provide a framework for directly addressing the frustration in phys…
The assembly of filamentous bundles with controlled diameters is common in biological systems and desirable for the development of nanomaterials. We discuss dynamical simulations and free energy calculations on patchy spheres with chiral pair interactions that spontaneously assemble into filamentous bundles. The chirality frustrates long-range crystal order by introducing twist between interacting subunits. For some ranges of system parameters this constraint leads to bundles with a finite diameter as the equilibrium state, and in other cases frustration is relieved by the formation of defects…
It is generally understood that geometric frustration prevents maximal hexagonal packings in uniform filament bundles upon twist. We demonstrate that a hexagonal packed elastic filament bundle can preserve its order over a wide range of twist due to a subtle counteraction of geometric expansion with elastic contraction. Using x-ray scanning and by locating each filament in the bundle, we show the remarkable persistence of order even as the twist is increased well above 360 degrees, by measuring the spatial correlation function across the bundle crosssection. We introduce a model which analyzes…
Geometric frustration results from a discrepancy between the locally favored arrangement of the constituents of a system and the geometry of the embedding space. Geometric frustration can be either non-cumulative, which implies an extensive energy growth, or cumulative which implies super-extensive energy scaling and highly cooperative ground state configurations which may depend on the dimensions of the system. Cumulative geometric frustration was identified in a variety of continuous systems including liquid crystals, filament bundles and molecular crystals. However, a spin-lattice model whi…
We examine the mechanism of bundling of cytoskeletal actin filaments by two representative bundling proteins, fascin and espin. Small-angle X-ray studies show that increased binding from linkers drives a systematic \textit{overtwist} of actin filaments from their native state, which occurs in a linker-dependent fashion. Fascin bundles actin into a continuous spectrum of intermediate twist states, while espin only allows for untwisted actin filaments and fully-overtwisted bundles. Based on a coarse-grained, statistical model of protein binding, we show that the interplay between binding geometr…
The actin cytoskeleton is a key component in the machinery of eukaryotic cells, and it selfassembles out of equilibrium into a wide variety of biologically crucial structures. While the molecular mechanisms involved are well characterized, the physical principles governing the spatial arrangement of actin filaments are not understood. Here we propose that the dynamics of actin network assembly from growing filaments results from a competition between diffusion, bundling, and steric hindrance, and is responsible for the range of observed morphologies. Our model and simulations thus predict an a…
The uniform director field obtained for the nematic ground state of the hard-rod model of liquid crystals in two dimensions reflects the high symmetry of the constituents of the liquid; It is a manifestation of the constituents' local tendency to avoid splaying and bending with respect to one another. In contrast, bent-core (or banana shaped) liquid-crystal-forming-molecules locally favor a state of zero splay and constant bend. However, such a structure cannot be realized in the plane and the resulting liquid-crystalline phase is frustrated and must exhibit some compromise of these two mutual…
Controlling the self-assembly of supramolecular structures is vital for living cells, and a central challenge for engineering at the nano- and microscales. Nevertheless, even particles without optimized shapes can robustly form well-defined morphologies. This is the case in numerous medical conditions where normally soluble proteins aggregate into fibers. Beyond the diversity of molecular mechanisms involved, we propose that fibers generically arise from the aggregation of irregular particles with short-range interactions. Using a minimal model of ill-fitting, sticky particles, we demonstrate …
Helical structures are ubiquitous in nature and engineering, ranging from DNA molecules to plant tendrils, from sea snail shells to nanoribbons. While the helical shapes in natural and engineered systems often exhibit nearly uniform radius and pitch, helical shell structures with changing radius and pitch, such as seashells and some plant tendrils, adds to the variety of this family of aesthetic beauty. Here we develop a comprehensive theoretical framework for tunable helical morphologies, and report the first biomimetic seashell-like structure resulting from mechanics of geometric frustration…
Molecular chirality frustrates the two-dimensional assembly of filamentous molecules, a fact that reflects the generic impossibility of imposing a global twisting of layered materials. We explore the consequences of this frustration for hexagonally-ordered assemblies of chiral filaments that are {\it finite} in lateral dimension. Specifically, we employ a continuum-elastic description of cylindrical bundles of filaments, allowing us to consider the most general resistance to and preference for chiral ordering of the assembly. We explore two distinct mechanisms by which chirality at the molecul…
Soft elastic filaments that can be stretched, bent and twisted exhibit a range of topologically and geometrically complex morphologies that include plectonemes, solenoids, knot-like and braid-like structures. We combine numerical simulations of soft elastic filaments that account for geometric nonlinearities and self-contact to map out these structures in a phase diagram that is a function of extension and twist density, consistent with previous experimental observations. By using ideas from computational topology, we also track the interconversion of link, twist and writhe in these geometrica…
Twisted and rope-like assemblies of filamentous molecules are common and vital structural elements in cells and tissue of living organisms. We study the intrinsic frustration occurring in these materials between the two-dimensional organization of filaments in cross section and out-of-plane interfilament twist in bundles. Using non-linear continuum elasticity theory of columnar materials, we study the favorable coupling of twist-induced stresses to the presence of edge dislocations in the lattice packing of bundles, which leads to a restructuring of the ground-state order of these materials at…
Filamentous bacteriophages such as fd-like viruses are monodisperse rod-like colloids that have well defined properties: diameter, length, rigidity, charge and chirality. Engineering those viruses leads to a library of colloidal rods which can be used as building blocks for reconfigurable and hierarchical self-assembly. Their condensation in aqueous solution þ{with additive polymers which act as depletants to induce} attraction between the rods leads to a myriad of fluid-like micronic structures ranging from isotropic/nematic droplets, colloid membranes, achiral membrane seeds, twisted ribbons…
The occurrence of coiled or helical morphologies is common in nature, from plant roots to DNA packaging into viral capsids, as well as in applications such as oil drilling processes. In many examples, chiral structures result from the buckling of a straight fiber either with intrinsic twist or to which end moments have been applied in addition to compression forces. Here, we elucidate a generic way to form regular helicoidal shapes from achiral straight filaments transported in viscous flows with free ends. Through a combination of experiments using fluorescently labeled actin filaments in mic…
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…
This perspective will overview an emerging paradigm for self-organized soft materials, {\it geometrically-frustrated assemblies}, where interactions between self-assembling elements (e.g. particles, macromolecules, proteins) favor local packing motifs that are incompatible with uniform global order in the assembly. This classification applies to a broad range of material assemblies including self-twisting protein filament bundles, amyloid fibers, chiral smectics and membranes, particle-coated droplets, curved protein shells and phase-separated lipid vesicles. In assemblies, geometric frustrati…
Living cells dynamically modulate the local morphologies of their actin cytoskeletons to perform biological functions, including force transduction, intracellular transport, and cell division. A major challenge is to understand how diverse structures of the actin cytoskeleton are assembled from a limited set of molecular building blocks. Here we study the spontaneous self-assembly of a minimal model of cytoskeletal materials, consisting of semiflexible actin filaments, crosslinkers, and molecular motors. Using coarse-grained simulations, we demonstrate that by changing concentrations and kinet…
