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Title: Valence-programmable nanoparticle architectures

Abstract

Abstract Nanoparticle-based clusters permit the harvesting of collective and emergent properties, with applications ranging from optics and sensing to information processing and catalysis. However, existing approaches to create such architectures are typically system-specific, which limits designability and fabrication. Our work addresses this challenge by demonstrating that cluster architectures can be rationally formed using components with programmable valence. We realize cluster assemblies by employing a three-dimensional (3D) DNA meshframe with high spatial symmetry as a site-programmable scaffold, which can be prescribed with desired valence modes and affinity types. Thus, this meshframe serves as a versatile platform for coordination of nanoparticles into desired cluster architectures. Using the same underlying frame, we show the realization of a variety of preprogrammed designed valence modes, which allows for assembling 3D clusters with complex architectures. The structures of assembled 3D clusters are verified by electron microcopy imaging, cryo-EM tomography and in-situ X-ray scattering methods. We also find a close agreement between structural and optical properties of designed chiral architectures.

Authors:
ORCiD logo; ORCiD logo; ORCiD logo; ; ; ; ORCiD logo
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:
1782014
Alternate Identifier(s):
OSTI ID: 1635470
Report Number(s):
BNL-216080-2020-JAAM
Journal ID: ISSN 2041-1723; 2279; PII: 16157
Grant/Contract Number:  
SC0012704
Resource Type:
Published Article
Journal Name:
Nature Communications
Additional Journal Information:
Journal Name: Nature Communications Journal Volume: 11 Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United Kingdom
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Sun, Sha, Yang, Shize, Xin, Huolin L., Nykypanchuk, Dmytro, Liu, Mingzhao, Zhang, Honghu, and Gang, Oleg. Valence-programmable nanoparticle architectures. United Kingdom: N. p., 2020. Web. https://doi.org/10.1038/s41467-020-16157-0.
Sun, Sha, Yang, Shize, Xin, Huolin L., Nykypanchuk, Dmytro, Liu, Mingzhao, Zhang, Honghu, & Gang, Oleg. Valence-programmable nanoparticle architectures. United Kingdom. https://doi.org/10.1038/s41467-020-16157-0
Sun, Sha, Yang, Shize, Xin, Huolin L., Nykypanchuk, Dmytro, Liu, Mingzhao, Zhang, Honghu, and Gang, Oleg. Fri . "Valence-programmable nanoparticle architectures". United Kingdom. https://doi.org/10.1038/s41467-020-16157-0.
@article{osti_1782014,
title = {Valence-programmable nanoparticle architectures},
author = {Sun, Sha and Yang, Shize and Xin, Huolin L. and Nykypanchuk, Dmytro and Liu, Mingzhao and Zhang, Honghu and Gang, Oleg},
abstractNote = {Abstract Nanoparticle-based clusters permit the harvesting of collective and emergent properties, with applications ranging from optics and sensing to information processing and catalysis. However, existing approaches to create such architectures are typically system-specific, which limits designability and fabrication. Our work addresses this challenge by demonstrating that cluster architectures can be rationally formed using components with programmable valence. We realize cluster assemblies by employing a three-dimensional (3D) DNA meshframe with high spatial symmetry as a site-programmable scaffold, which can be prescribed with desired valence modes and affinity types. Thus, this meshframe serves as a versatile platform for coordination of nanoparticles into desired cluster architectures. Using the same underlying frame, we show the realization of a variety of preprogrammed designed valence modes, which allows for assembling 3D clusters with complex architectures. The structures of assembled 3D clusters are verified by electron microcopy imaging, cryo-EM tomography and in-situ X-ray scattering methods. We also find a close agreement between structural and optical properties of designed chiral architectures.},
doi = {10.1038/s41467-020-16157-0},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United Kingdom},
year = {2020},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41467-020-16157-0

Figures / Tables:

Figure 1 Figure 1: Schematic of nanoparticle-cluster self-assembly directed by the valence-programmable pentakis icosidodecahedron DNA meshframe. a. Conceptual illustration of a nanoparticle (NP) cluster coordinated by sphere-like frame structure with arbitrarily prescribed valence modes and different types of binding affinities (shown as colors). Designated vertices provide binding affinities to corresponding DNA-encoded NPsmore » (shown with matched colors). b. Designed DNA meshframe origami, pentakis icosidodecahedron (grey skeleton), for programming designed NP cluster architectures. Zoomed-in vertex shows that it is formed by six edges, with each edge consisting of one double helix. Dark grey lines indicate staple strands and light grey lines indicate a templating DNA. The DNA meshframe can be encoded by introducing ssDNA around the vertex. An encoded vertex is zoomed in to show that six identical sticky ends (green curves) protrude from a designated vertex. Sticky ends anchored on designated vertices form valence modes of triangular bipyramid and helix (top and middle). Distinctive sets of sticky ends (strands with different colors) can be anchored at designated vertices (middle and bottom). NPs (red balls), capped with complementary DNA shells, are assembled into designed clusters through their coordination around the meshframe corresponding with the programmed vertices, for example (from top to bottom): symmetric nanocluster, arbitrary prescribed nanocluster with chiral helical valence mode, and multi-type NP cluster.« less

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