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Title: The Stability of a Nanoparticle Diamond Lattice Linked by DNA

Abstract

The functionalization of nanoparticles (NPs) with DNA has proven to be an effective strategy for self-assembly of NPs into superlattices with a broad range of lattice symmetries. By combining this strategy with the DNA origami approach, the possible lattice structures have been expanded to include the cubic diamond lattice. This symmetry is of particular interest, both due to the inherent synthesis challenges, as well as the potential valuable optical properties, including a complete band-gap. Using these lattices in functional devices requires a robust and stable lattice. Here, we use molecular simulations to investigate how NP size and DNA stiffness affect the structure, stability, and crystallite shape of NP superlattices with diamond symmetry. We use the Wulff construction method to predict the equilibrium crystallite shape of the cubic diamond lattice. We find that, due to reorientation of surface particles, it is possible to create bonds at the surface with dangling DNA links on the interior, thereby reducing surface energy. Consequently, the crystallite shape depends on the degree to which such surface reorientation is possible, which is sensitive to DNA stiffness. Further, we determine dependence of the lattice stability on NP size and DNA stiffness by evaluating relative Gibbs free energy. Wemore » find that the free energy is dominated by the entropic component. Increasing NP size or DNA stiffness increases free energy, and thus decreases the relative stability of lattices. On the other hand, increasing DNA stiffness results in a more precisely defined lattice structure. Thus, there is a trade off between structure and stability of the lattice. Our findings should assist experimental design for controlling lattice stability and crystallite shape.« less

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]
  1. Wesleyan Univ., Middelton, CT (United States). Dept. of Physics; Columbia Univ., New York, NY (United States). Dept. of Applied Physics and Applied Mathematics
  2. Columbia Univ., New York, NY (United States). Dept. of Applied Physics and Applied Mathematics; Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
  3. Wesleyan Univ., Middelton, CT (United States). Dept. of Physics; Wesleyan Univ., Middelton, CT (United States). Dept. of Molecular Biology & Biochemistry
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1562479
Report Number(s):
BNL-212088-2019-JAAM
Journal ID: ISSN 2079-4991; NANOKO
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nanomaterials
Additional Journal Information:
Journal Volume: 9; Journal Issue: 5; Journal ID: ISSN 2079-4991
Publisher:
MDPI
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; 77 NANOSCIENCE AND NANOTECHNOLOGY; DNA nanotechnology; self-assembly; nanoparticle superlattice

Citation Formats

Emamy, Hamed, Gang, Oleg, and Starr, Francis W. The Stability of a Nanoparticle Diamond Lattice Linked by DNA. United States: N. p., 2019. Web. doi:10.3390/nano9050661.
Emamy, Hamed, Gang, Oleg, & Starr, Francis W. The Stability of a Nanoparticle Diamond Lattice Linked by DNA. United States. doi:10.3390/nano9050661.
Emamy, Hamed, Gang, Oleg, and Starr, Francis W. Fri . "The Stability of a Nanoparticle Diamond Lattice Linked by DNA". United States. doi:10.3390/nano9050661. https://www.osti.gov/servlets/purl/1562479.
@article{osti_1562479,
title = {The Stability of a Nanoparticle Diamond Lattice Linked by DNA},
author = {Emamy, Hamed and Gang, Oleg and Starr, Francis W.},
abstractNote = {The functionalization of nanoparticles (NPs) with DNA has proven to be an effective strategy for self-assembly of NPs into superlattices with a broad range of lattice symmetries. By combining this strategy with the DNA origami approach, the possible lattice structures have been expanded to include the cubic diamond lattice. This symmetry is of particular interest, both due to the inherent synthesis challenges, as well as the potential valuable optical properties, including a complete band-gap. Using these lattices in functional devices requires a robust and stable lattice. Here, we use molecular simulations to investigate how NP size and DNA stiffness affect the structure, stability, and crystallite shape of NP superlattices with diamond symmetry. We use the Wulff construction method to predict the equilibrium crystallite shape of the cubic diamond lattice. We find that, due to reorientation of surface particles, it is possible to create bonds at the surface with dangling DNA links on the interior, thereby reducing surface energy. Consequently, the crystallite shape depends on the degree to which such surface reorientation is possible, which is sensitive to DNA stiffness. Further, we determine dependence of the lattice stability on NP size and DNA stiffness by evaluating relative Gibbs free energy. We find that the free energy is dominated by the entropic component. Increasing NP size or DNA stiffness increases free energy, and thus decreases the relative stability of lattices. On the other hand, increasing DNA stiffness results in a more precisely defined lattice structure. Thus, there is a trade off between structure and stability of the lattice. Our findings should assist experimental design for controlling lattice stability and crystallite shape.},
doi = {10.3390/nano9050661},
journal = {Nanomaterials},
number = 5,
volume = 9,
place = {United States},
year = {2019},
month = {4}
}

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