Possibilities and limits of DNA-enabled programmable 2D self-assembly

Programmable self-assembly provides a promising avenue to improve upon traditional synthesis and create multi-component materials with emergent properties and arbitrary nanoscale complexity. However, its most successful realizations utilizing DNA often use complicated arduous procedures that result in low yields. Here, we employ coarse-grained molecular dynamics to uncover the ranges of temperatures and misbinding strengths needed for successful one-pot self-assembly of generic, two-dimensional (2D), and distinguishable blocks. Analysis of the energies associated with a single-stranded DNA interacting with all other sequences within a mixture revealed that the success of DNA-based assembly is primarily determined by the strongest misbinding a given sequence can encounter with a sequence highly similar to its reverse complement. This enabled us to design optimized sequence ensembles with acceptably weak and consequently rare misbinding. An estimate is provided for the maximum size of, and complexity of sequences needed to synthesize self-assembled structures with high accuracy and yield, with potential relevance for DNA-functionalized low-dimensional materials for electronics and energy storage.