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Title: Design strategies for self-assembly of discrete targets

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 ismore » a priority.« less

Authors:
Publication Date:
OSTI Identifier:
22493474
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 143; Journal Issue: 4; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; COMPARATIVE EVALUATIONS; COMPUTERIZED SIMULATION; DIAGRAMS; DIFFUSION; MATHEMATICAL MODELS; MONTE CARLO METHOD; NAVIER-STOKES EQUATIONS; PARTICLES; SOLID CLUSTERS; TRAJECTORIES

Citation Formats

Madge, Jim, and Miller, Mark A., E-mail: m.a.miller@durham.ac.uk. Design strategies for self-assembly of discrete targets. United States: N. p., 2015. Web. doi:10.1063/1.4927671.
Madge, Jim, & Miller, Mark A., E-mail: m.a.miller@durham.ac.uk. Design strategies for self-assembly of discrete targets. United States. https://doi.org/10.1063/1.4927671
Madge, Jim, and Miller, Mark A., E-mail: m.a.miller@durham.ac.uk. 2015. "Design strategies for self-assembly of discrete targets". United States. https://doi.org/10.1063/1.4927671.
@article{osti_22493474,
title = {Design strategies for self-assembly of discrete targets},
author = {Madge, Jim and Miller, Mark A., E-mail: m.a.miller@durham.ac.uk},
abstractNote = {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.},
doi = {10.1063/1.4927671},
url = {https://www.osti.gov/biblio/22493474}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 4,
volume = 143,
place = {United States},
year = {Tue Jul 28 00:00:00 EDT 2015},
month = {Tue Jul 28 00:00:00 EDT 2015}
}