Temperature Protocols to Guide Selective Self-Assembly of Competing Structures

TL;DR

This paper presents a method for designing multi-component self-assembly systems that can selectively form one of two competing structures using simple temperature protocols, enabling on-demand reconfiguration.

Contribution

It introduces principles for inverse design of self-assembly mixtures capable of selectively encoding and retrieving two structures via temperature control, highlighting minimal shared components and nucleation barriers.

Findings

Temperature protocols enable selective formation of target structures.

Minimal shared neighboring pairs reduce chimeric aggregates.

Design strategies improve reconfigurability of self-assembly systems.

Abstract

Multi-component self-assembly mixtures offer the possibility of encoding multiple target structures with the same set of interacting components. Selective retrieval of one of the stored structures has been attempted by preparing an initial state that favours the assembly of the required target, through seeding, concentration patterning or specific choices of interaction strengths. This may not be possible in an experiment where on-the-fly reconfiguration of the building blocks to switch functionality may be required. In this paper, we explore principles of inverse design of a multi-component self-assembly mixture capable of encoding two competing structures that can be selected through simple temperature protocols. We design the target structures to realise the generic situation in which one of targets has the lower nucleation barrier while the other is globally more stable. We observe that to avoid the formation of spurious or chimeric aggregates, the number of neighbouring component pairs that occur in both structures should be minimal. Our design also requires the inclusion of components that are part only of one of the target structures, but we observe that to maximize the selectivity of retrieval, the component library itself should be maximally shared by the two targets. We demonstrate that temperature protocols can be designed which lead to the formation of either one of the target structures with high selectivity. We discuss the important role played by secondary aggregation products, which we term vestigial aggregates.