2025 Theses Doctoral

Engineering DNA-mediated interactions between self-assembling building blocks for nanomaterial fabrication

McKeen, Daniel

Recent developments in DNA-mediated self-assembly strategies present powerful opportunities for not only furthering fundamental understanding of how to design and organize nanomaterials but also developing a robust nanomaterial fabrication platform. This dissertation will discuss how engineering the DNA-based interactions between nanoscale building blocks can fabricate nanomaterials with complex crystalline symmetries and stimuli-responsive capabilities.

I cover the state of the DNA-mediated self-assembly field in Chapter 1. After, in Chapter 2, I will discuss engineering DNA interactions between isotropic spherical nanoparticle shells to prescribe interparticle pair potentials that subsequently controls nanomaterial crystal phase. In Chapter 3, I share work with DNA origami frames that serve as programmable “material voxels” and our investigation and manipulation of their assembly pathway. I describe a novel workflow for nanomaterial fabrication that relies on an SAT solver and our material voxel in Chapter 4.

In Chapters 5 and 6, I describe our efforts to integrate stimuli-responsive properties into our DNA nanomaterials. Chapter 5 focuses on our efforts integrating enzymatic agents to drive assembly, disassembly, and re-organization of DNA nanomaterials. Chapter 6 focuses on co-assembly of our DNA-based assemblies with magnetic supports to realize magnetically responsive nanomaterials. In Chapter 7, I discuss the overall dissertation and the future outlook for developments in the field of DNA-mediated self-assembly.