Molecular engineering of chiral colloidal liquid crystals using DNA origami

Establishing precise control over the shape and the interactions of the microscopic building blocks is essential for design of macroscopic soft materials with novel structural, optical and mechanical properties. Here, we demonstrate robust assembly of DNA origami filaments into cholesteric liquid crystals, 1D supramolecular twisted ribbons and 2D colloidal membranes. The exquisite control afforded by the DNA origami technology establishes a quantitative relationship between the microscopic filament structure and the macroscopic cholesteric pitch. Furthermore, it also enables robust assembly of 1D twisted ribbons, which behave as effective supramolecular polymers whose structure and elastic properties can be precisely tuned by controlling the geometry of the elemental building blocks. Our results demonstrate the potential synergy between DNA origami technology and colloidal science, in which the former allows for rapid and robust synthesis of complex particles, and the latter can be used to assemble such particles into bulk materials

Robust Procedures for Obtaining Assembly Contact State Extremal Configurations

Two important components in the selection of an admittance that facilitates force-guided assembly are the identification of: 1) the set of feasible contact states, and 2) the set of configurations that span each contact state, i.e., the extremal configurations. We present a procedure to automatically generate both sets from CAD models of the assembly parts. In the procedure, all possible combinations of principle contacts are considered when generating hypothesized contact states. The feasibility of each is then evaluated in a genetic algorithm based optimization procedure. The maximum and minimum value of each of the 6 configuration variables spanning each contact state are obtained by again using genetic algorithms. Together, the genetic algorithm approach, the hierarchical data structure containing the states, the relationships among the states, and the extremals within each state are used to provide a reliable means of identifying all feasible contact states and their associated extremal configurations

Rethinking a Reinvigorated Right To Assemble

Revived after a decades-long slumber, the First Amendment’s Assembly Clause has garnered robust attention of late. Endeavoring to reinvigorate this forgotten clause, legal scholars have outlined a normative vision of the assembly right that would better safeguard the freedom of association. This Note argues that such an approach—no matter its merits or its deficiencies—overlooks the Clause’s central aim. The assembly right is in fact best understood as an assembly right, not as a right about associations. This Note advances that proposition by closely analyzing the text and the history of the Assembly Clause, a project that has not yet been systematically undertaken. The evidence unearthed from this inquiry demonstrates that the Assembly Clause seeks, as its first-order concern, to protect in-person, flesh–and–blood gatherings. Such protection is thus ultimately of great import in rethinking both the freedoms afforded and the constraints imposed on dissent within our constitutional framework

Programmable Control of Nucleation for Algorithmic Self-Assembly

Algorithmic self-assembly, a generalization of crystal growth processes, has been proposed as a mechanism for autonomous DNA computation and for bottom-up fabrication of complex nanostructures. A `program' for growing a desired structure consists of a set of molecular `tiles' designed to have specific binding interactions. A key challenge to making algorithmic self-assembly practical is designing tile set programs that make assembly robust to errors that occur during initiation and growth. One method for the controlled initiation of assembly, often seen in biology, is the use of a seed or catalyst molecule that reduces an otherwise large kinetic barrier to nucleation. Here we show how to program algorithmic self-assembly similarly, such that seeded assembly proceeds quickly but there is an arbitrarily large kinetic barrier to unseeded growth. We demonstrate this technique by introducing a family of tile sets for which we rigorously prove that, under the right physical conditions, linearly increasing the size of the tile set exponentially reduces the rate of spurious nucleation. Simulations of these `zig-zag' tile sets suggest that under plausible experimental conditions, it is possible to grow large seeded crystals in just a few hours such that less than 1 percent of crystals are spuriously nucleated. Simulation results also suggest that zig-zag tile sets could be used for detection of single DNA strands. Together with prior work showing that tile sets can be made robust to errors during properly initiated growth, this work demonstrates that growth of objects via algorithmic self-assembly can proceed both efficiently and with an arbitrarily low error rate, even in a model where local growth rules are probabilistic.Comment: 37 pages, 14 figure

Reducing facet nucleation during algorithmic self-assembly

Algorithmic self-assembly, a generalization of crystal growth, has been proposed as a mechanism for bottom-up fabrication of complex nanostructures and autonomous DNA computation. In principle, growth can be programmed by designing a set of molecular tiles with binding interactions that enforce assembly rules. In practice, however, errors during assembly cause undesired products, drastically reducing yields. Here we provide experimental evidence that assembly can be made more robust to errors by adding redundant tiles that "proofread" assembly. We construct DNA tile sets for two methods, uniform and snaked proofreading. While both tile sets are predicted to reduce errors during growth, the snaked proofreading tile set is also designed to reduce nucleation errors on crystal facets. Using atomic force microscopy to image growth of proofreading tiles on ribbon-like crystals presenting long facets, we show that under the physical conditions we studied the rate of facet nucleation is 4-fold smaller for snaked proofreading tile sets than for uniform proofreading tile sets