Sliding across a surface: Particles with fixed and mobile ligands.

A quantitative model of the mobility of ligand-presenting particles at the interface is pivotal to understanding important systems in biology and nanotechnology. In this work, we investigate the emerging dynamics of particles featuring ligands that selectively bind receptors decorating an interface. The formation of a ligand-receptor complex leads to a molecular bridge anchoring the particle to the surface. We consider systems with reversible bridges in which ligand-receptor pairs bind/unbind with finite reaction rates. For a given set of bridges, the particle can explore a tiny fraction of the surface as the extensivity of the bridges is finite. We show how, at timescales longer than the bridges' lifetime, the average position of the particle diffuses away from its initial value. We distill our findings into two analytic equations for the sliding diffusion constant of particles carrying mobile and fixed ligands. We quantitatively validate our theoretical predictions using reaction-diffusion simulations. We compare our findings with results from recent literature studies and discuss the molecular parameters that likely affect the particle's mobility most. Our results, along with recent literature studies, will allow inferring the microscopic parameters at play in complex biological systems from experimental trajectories.

Self-Assembly and Crystallization of DNA-Coated Colloids via Linker-Encoded Interactions.

Coating colloidal particles with DNA is a promising strategy to make functional nanoscale materials because the particles can be programmed to spontaneously self-assemble into complex, ordered structures. In this Article, we explore the phase behavior and types of structures that can be formed when interactions between DNA-coated colloids are specified by linker DNA strands dispersed in solution. We show that linker-mediated interactions direct the self-assembly of colloids into equilibrium crystal structures. Furthermore, we demonstrate how different linker sequences and concentrations produce different crystal lattices, whose symmetry and compositional order are encoded exclusively by the linker-mediated interactions. These results illustrate how linkers can be used to separate the assembly instructions, encoded in the linkers, from the colloids themselves. We also examine the phase behavior of asymmetric linkers, which bind more strongly to one colloidal species than the other. We find that asymmetry strongly influences the concentration dependence of the colloidal interactions, which we explain using a mean-field model. We also find evidence that asymmetric linkers might help to reduce kinetic bottlenecks to colloidal crystallization. Together, our findings expand the design rules of linker-mediated self-assembly and make connections between the various schemes for programming assembly of DNA-coated colloids reported in the literature.

The role of deformability in determining the structural and mechanical properties of bubbles and emulsions.

We perform computational studies of jammed particle packings in two dimensions undergoing isotropic compression using the well-characterized soft particle (SP) model and deformable particle (DP) model that we developed for bubbles and emulsions. In the SP model, circular particles are allowed to overlap, generating purely repulsive forces. In the DP model, particles minimize their perimeter, while deforming at fixed area to avoid overlap during compression. We compare the structural and mechanical properties of jammed packings generated using the SP and DP models as a function of the packing fraction ρ, instead of the reduced number density φ. We show that near jamming onset the excess contact number Δz = z - zJ and shear modulus G scale as Δρ0.5 in the large system limit for both models, where Δρ = ρ - ρJ and zJ ≈ 4 and ρJ ≈ 0.842 are the values at jamming onset. Δz and G for the SP and DP models begin to differ for ρ ⪆ 0.88. In this regime, Δz ∼ G can be described by a sum of two power-laws in Δρ, i.e. Δz ∼ G ∼ C0Δρ0.5 + C1Δρ1.0 to lowest order. We show that the ratio C1/C0 is much larger for the DP model compared to that for the SP model. We also characterize the void space in jammed packings as a function of ρ. We find that the DP model can describe the formation of Plateau borders as ρ → 1. We further show that the results for z and the shape factor A versus ρ for the DP model agree with recent experimental studies of foams and emulsions.

Universal scaling of polygonal desiccation crack patterns.

Polygonal desiccation crack patterns are commonly observed in natural systems. Despite their quotidian nature, it is unclear whether similar crack patterns which span orders of magnitude in length scales share the same underlying physics. In thin films, the characteristic length of polygonal cracks is known to monotonically increase with the film thickness; however, existing theories that consider the mechanical, thermodynamic, hydrodynamic, and statistical properties of cracking often lead to contradictory predictions. Here we experimentally investigate polygonal cracks in drying suspensions of micron-sized particles by varying film thickness, boundary adhesion, packing fraction, and solvent. Although polygonal cracks were observed in most systems above a critical film thickness, in cornstarch-water mixtures, multiscale crack patterns were observed due to two distinct desiccation mechanisms. Large-scale, primary polygons initially form due to capillary-induced film shrinkage, whereas small-scale, secondary polygons appear later due to the deswelling of the hygroscopic particles. In addition, we find that the characteristic area of the polygonal cracks, A_{p}, obeys a universal power law, A_{p}=αh^{4/3}, where h is the film thickness. By quantitatively linking α with the material properties during crack formation, we provide a robust framework for understanding multiscale polygonal crack patterns from microscopic to geologic scales.