Colloidal Layer Deposition with a Controllable Number of Layers and Compositional Order

We design a system with a binary suspension of colloids and a surface that triggers the self-assembly of crystallites with a finite thickness. The proposed design allows controlling the number of layers forming the aggregate and constrains the two types of particles to lie on different planes. These functionalities are achieved by decorating the colloids and the surface with multiple DNA oligomers featuring specific interactions. Similarly to what was proposed in previous studies, the surface triggers a chain of reactions between DNA oligomers, leading to localized self-assembly. System parameters control the thickness of the aggregates. In this work, compositional order is achieved by engineering the reaction kinetics between DNA oligomers in a way that limits interactions between colloids of the same type. We validate our design using theory and reaction-diffusion simulation algorithms, which capture the multibody nature of the interactions. This work demonstrates how engineering the reaction kinetics provides a new tool for controlling the morphology of aggregates assembled by DNA.