title: Sequential programmable self-assembly: Role of cooperative interactions.
abstract: We propose a general strategy of "sequential programmable self-assembly" that enables a bottom-up design of arbitrary multi-particle architectures on nano- and microscales. We show that a naive realization of this scheme, based on the pairwise additive interactions between particles, has fundamental limitations that lead to a relatively high error rate. This can be overcome by using cooperative interparticle binding. The cooperativity is a well known feature of many biochemical processes, responsible, e.g., for signaling and regulations in living systems. Here we propose to utilize a similar strategy for high precision self-assembly, and show that DNA-mediated interactions provide a convenient platform for its implementation. In particular, we outline a specific design of a DNA-based complex which we call "DNA spider," that acts as a smart interparticle linker and provides a built-in cooperativity of binding. We demonstrate versatility of the sequential self-assembly based on spider-functionalized particles by designing several mesostructures of increasing complexity and simulating their assembly process. This includes a number of finite and repeating structures, in particular, the so-called tetrahelix and its several derivatives. Due to its generality, this approach allows one to design and successfully self-assemble virtually any structure made of a "GEOMAG" magnetic construction toy, out of nanoparticles. According to our results, once the binding cooperativity is strong enough, the sequential self-assembly becomes essentially error-free.
authors.affiliation: Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, USA.
authors.forename: Jonathan D
authors.initials: JD
authors.lastname: Halverson
authors.affiliation: Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, USA.
authors.forename: Alexei V
authors.initials: AV
authors.lastname: Tkachenko
mesh_terms: D004247:DNA / Q000737:chemistry*; D008962:Models, Theoretical; D009690:Nucleic Acid Conformation
chemical_list: D004247:DNA