DNA Origami Crystals: Effects of Design Parameters on Self-Assembly Kinetics

Programmable self-assembly of nanoparticles into ordered 3D frameworks offers a promising route for nanoscale materials design. To achieve this, DNA-based polyhedral motifs with sequence-encoded interactions are commonly used to enable selective, directional binding between components. These DNA-origami building blocks allow for many tunable design choices, such as the motif geometry, interaction multiplicity (number of unique binding sequences per component), and sticky-end sequences, which govern the binding interactions between components. However, the effects of these design choices on the kinetics of self-assembly remain poorly understood. Here, we perform coarse-grained molecular dynamics simulations using patchy-particle models parameterized according to these design choices. We validate the predictions of these models with experiments by computing dimerization equilibrium constants and phase diagrams for four families of multicomponent lattice structures of varying complexity. We then use these simulations to investigate the consequences of various design choices for the self-assembly kinetics of the four lattice structures. These results provide insight into how design parameters and interaction specificity influence both the phase behavior and self-assembly kinetics of multicomponent materials of varying structural complexity.