Tunable Patterning of DNA Origami on Surfaces Using Steric Brushes

Tailoring the properties of 2D materials through precise control of both local arrangement and long-range order on surfaces remains a central challenge in materials science. While surface-assisted assembly of symmetric, non-interacting DNA origami nanostructures offers a facile route to 2D superlattices, existing approaches typically yield close-packed arrays with limited control over inter-origami spacing. Here, we present a tunable and reproducible strategy for regulating the lateral spacing of DNA origami during self-assembly into macroscopic 2D lattice patterns. By controlling the growth of uniform single-stranded polynucleotide brushes from the surface of DNA origami, we modulate their effective geometry by introducing longer-ranged entropic repulsion, which enables precise and adjustable control over inter-origami distances across macroscopic areas. Using integrated experiments and simulations, we demonstrate how systematic variation of brush length, surface adsorption strength, and brush density can lead to tunable surface patterns across different origami shapes. Overall, this straightforward approach advances the field of DNA-templated nanofabrication by providing highly programmable templates with precise spatial control. This platform offers a robust foundation for the future integration of functional nanomaterials and the development of organized nanostructures.