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Title: Sequential programmable self-assembly: Role of cooperative interactions

Abstract

Here, 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 ofmore » nanoparticles. According to our results, once the binding cooperativity is strong enough, the sequential self-assembly becomes essentially error-free.« less

Authors:
;  [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1255731
Alternate Identifier(s):
OSTI ID: 1421159
Report Number(s):
BNL-112267-2016-JA
Journal ID: ISSN 0021-9606; KC0403020
Grant/Contract Number:  
SC00112704; SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 144; Journal Issue: 9; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; self assembly; DNA; free energy; bond formation; colloidal systems

Citation Formats

Jonathan D. Halverson, and Tkachenko, Alexei V.. Sequential programmable self-assembly: Role of cooperative interactions. United States: N. p., 2016. Web. https://doi.org/10.1063/1.4942615.
Jonathan D. Halverson, & Tkachenko, Alexei V.. Sequential programmable self-assembly: Role of cooperative interactions. United States. https://doi.org/10.1063/1.4942615
Jonathan D. Halverson, and Tkachenko, Alexei V.. Fri . "Sequential programmable self-assembly: Role of cooperative interactions". United States. https://doi.org/10.1063/1.4942615. https://www.osti.gov/servlets/purl/1255731.
@article{osti_1255731,
title = {Sequential programmable self-assembly: Role of cooperative interactions},
author = {Jonathan D. Halverson and Tkachenko, Alexei V.},
abstractNote = {Here, 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.},
doi = {10.1063/1.4942615},
journal = {Journal of Chemical Physics},
number = 9,
volume = 144,
place = {United States},
year = {2016},
month = {3}
}

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