On Kinetic Constraints That Catalysis Imposes on Elementary Processes.

Catalysis, the acceleration of product formation by a substance that is left unchanged, typically results from multiple elementary processes, including diffusion of the reactants toward the catalyst, chemical steps, and release of the products. While efforts to design catalysts are often focused on accelerating the chemical reaction on the catalyst, catalysis is a global property of the catalytic cycle that involves all processes. These are controlled by both intrinsic parameters such as the composition and shape of the catalyst and extrinsic parameters such as the concentration of the chemical species at play.

Computational design of a minimal catalyst using colloidal particles with programmable interactions.

Catalysis, the acceleration of chemical reactions by molecules that are not consumed in the process, is essential to living organisms but remains absent in physical systems that aspire to emulate biological functionalities with artificial components. Here we demonstrate how to design a catalyst using spherical building blocks interacting programmable potentials, and show that a minimal catalyst design, a rigid dimer, can accelerate a ubiquitous elementary reaction, the cleaving of a bond. Combining coarse-grained molecular dynamics simulations and theory, and by comparing the mean reaction time for bond dissociation in the presence and absence of the catalyst, we derive geometrical and physical constraints for its design and determine the reaction conditions under which catalysis emerges in the system.

Self-assembly of emulsion droplets through programmable folding.

In the realm of particle self-assembly, it is possible to reliably construct nearly arbitrary structures if all the pieces are distinct, but systems with fewer flavours of building blocks have so far been limited to the assembly of exotic crystals. Here we introduce a minimal model system of colloidal droplet chains, with programmable DNA interactions that guide their downhill folding into specific geometries. Droplets are observed in real space and time, unravelling the rules of folding.

Programming Directed Motion with DNA-Grafted Particles.

Colloidal particles can be programmed to interact in complex ways by functionalizing them with DNA oligonucleotides. Adding DNA strand-displacement reactions to the system allows these interparticle interactions to respond to specific changes in temperature. We present the requirements for thermally driven directed motion of colloidal particles, and we explore how these conditions can be realized experimentally using strand-displacement reactions.

Natural Selection beyond Life? A Workshop Report.

Natural selection is commonly seen not just as an explanation for adaptive evolution, but as the inevitable consequence of "heritable variation in fitness among individuals". Although it remains embedded in biological concepts, such a formalisation makes it tempting to explore whether this precondition may be met not only in life as we know it, but also in other physical systems. This would imply that these systems are subject to natural selection and may perhaps be investigated in a biological framework, where properties are typically examined in light of their putative functions.

Spontaneous emergence of catalytic cycles with colloidal spheres.

Colloidal particles endowed with specific time-dependent interactions are a promising route for realizing artificial materials that have the properties of living ones. Previous work has demonstrated how this system can give rise to self-replication. Here, we introduce the process of colloidal catalysis, in which clusters of particles catalyze the creation of other clusters through templating reactions.

Mutation at Expanding Front of Self-Replicating Colloidal Clusters.

We construct a scheme for self-replicating square clusters of particles in two spatial dimensions, and validate it with computer simulations in a finite-temperature heat bath. We find that the self-replication reactions propagate through the bath in the form of Fisher waves. Our model reflects existing colloidal systems, but is simple enough to allow simulation of many generations and thereby the first study of evolutionary dynamics in an artificial system.

Multifarious assembly mixtures: systems allowing retrieval of diverse stored structures.

Self-assembly materials are traditionally designed so that molecular or mesoscale components form a single kind of large structure. Here, we propose a scheme to create "multifarious assembly mixtures," which self-assemble many different large structures from a set of shared components. We show that the number of multifarious structures stored in the solution of components increases rapidly with the number of different types of components.

Size limits of self-assembled colloidal structures made using specific interactions.

We establish size limitations for assembling structures of controlled size and shape out of colloidal particles with short-ranged interactions. Through simulations we show that structures with highly variable shapes made out of dozens of particles can form with high yield, as long as each particle in the structure binds only to the particles in their local environment. To understand this, we identify the excited states that compete with the ground-state structure and demonstrate that these excited states have a completely topological characterization, valid when the interparticle interactions are short-ranged.

Contact changes near jamming.

We probe the onset and effect of contact changes in soft harmonic particle packings which are sheared quasistatically. We find that the first contact changes are the creation or breaking of contacts on a single particle. We characterize the critical strain, statistics of breaking versus making a contact, and ratio of shear modulus before and after such events, and explain their finite size scaling relations.

Self-replicating colloidal clusters.

We construct schemes for self-replicating clusters of spherical particles, validated with computer simulations in a finite-temperature heat bath. Each particle has stickers uniformly distributed over its surface, and the rules for self-replication are encoded into the specificity and strength of interactions. Geometrical constraints imply that a compact cluster can copy itself only with help of a catalyst, a smaller cluster that increases the surface area to form a template.

Using shape anisotropy to toughen disordered nanoparticle assemblies.

Assemblies of disordered nanoparticles constitute an important class of materials that have numerous applications in energy conversion and storage, electronics, photonics, and sensing. One major roadblock that limits the widespread utilization of disordered nanoparticle assemblies (DNAs) is their poor damage tolerance; they fracture under small loads and, thus, have low toughness. The absence of fundamental understanding on the mechanical behavior and failure mechanism of disordered nanoparticle assemblies makes it even more challenging to develop new strategies to toughen these structures without compromising their mechanical strength.