Design strategies for self-assembly of discrete targets

Madge, Jim; Miller, Mark A.

Abstract

Both biological and artificial self-assembly processes can take place by a range of different schemes, from the successive addition of identical building blocks to hierarchical sequences of intermediates, all the way to the fully addressable limit in which each component is unique. In this paper, we introduce an idealized model of cubic particles with patterned faces that allows self-assembly strategies to be compared and tested. We consider a simple octameric target, starting with the minimal requirements for successful self-assembly and comparing the benefits and limitations of more sophisticated hierarchical and addressable schemes. Simulations are performed using a hybrid dynamical Monte Carlo protocol that allows self-assembling clusters to rearrange internally while still providing Stokes-Einstein-like diffusion of aggregates of different sizes. Our simulations explicitly capture the thermodynamic, dynamic, and steric challenges typically faced by self-assembly processes, including competition between multiple partially completed structures. Self-assembly pathways are extracted from the simulation trajectories by a fully extendable scheme for identifying structural fragments, which are then assembled into history diagrams for successfully completed target structures. For the simple target, a one-component assembly scheme is most efficient and robust overall, but hierarchical and addressable strategies can have an advantage under some conditions if high yield is a priority.

Citation

Madge, J., & Miller, M. A. (2015). Design strategies for self-assembly of discrete targets. The Journal of Chemical Physics, 143(4), Article 044905. https://doi.org/10.1063/1.4927671

• Journal Article Type: Article
• Acceptance Date: Jul 21, 2015
• Online Publication Date: Jul 31, 2015
• Publication Date: Jul 28, 2015
• Deposit Date: Aug 12, 2015
• Publicly Available Date: Sep 4, 2015
• Journal: Journal of Chemical Physics
• Print ISSN: 0021-9606
• Electronic ISSN: 1089-7690
• Publisher: American Institute of Physics
• Peer Reviewed: Peer Reviewed
• Volume: 143
• Issue: 4
• Article Number: 044905
• DOI: https://doi.org/10.1063/1.4927671
• Public URL: https://durham-repository.worktribe.com/output/1404238
• Related Public URLs: http://arxiv.org/abs/1508.02627