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Title: Ordered three-dimensional nanomaterials using DNA-prescribed and valence-controlled material voxels

Abstract

The ability to organize nanoscale objects into well-defined three-dimensional (3D) arrays can translate advances in nanoscale synthesis into targeted material fabrication. Despite successes in nanoparticle assembly, most extant methods are system specific and not fully compatible with biomolecules. As such, here, we report a platform for creating distinct 3D ordered arrays from different nanomaterials using DNA-prescribed and valence-controlled material voxels. These material voxels consist of 3D DNA frames that integrate nano-objects within their scaffold, thus enabling the object’s valence and coordination to be determined by the frame’s vertices, which can bind to each other through hybridization. Such DNA material voxels define the lattice symmetry through the spatially prescribed valence decoupling the 3D assembly process from the nature of the nanocomponents, such as their intrinsic properties and shapes. We show this by assembling metallic and semiconductor nanoparticles and also protein superlattices. We support the technological potential of such an assembly approach by fabricating light-emitting 3D arrays with diffraction-limited spectral purity and 3D enzymatic arrays with increased activity.

Authors:
 [1];  [2]; ORCiD logo [3];  [4]; ORCiD logo [2]; ORCiD logo [3];  [5];  [5];  [2];  [4];  [4];  [4];  [4]; ORCiD logo [6]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Nanjing Univ. (China)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  3. Van Andel Inst., Grand Rapids, MI (United States)
  4. Columbia Univ., New York, NY (United States)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source
  6. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Columbia Univ., New York, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
Jiangsu Youth Fund of China; Fundamental Research Funds for the Central Universities (China); National Institutes of Health (NIH); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
OSTI Identifier:
1600469
Report Number(s):
BNL-213632-2020-JAAM
Journal ID: ISSN 1476-1122
Grant/Contract Number:  
SC0012704; BK20180337; 14380151; GM111472; GM124170; SC0008772
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 19; Journal Issue: 7; Journal ID: ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; Nanoparticles; Nanoscale materials; Organizing materials with DNA; Self-assembly

Citation Formats

Tian, Ye, Lhermitte, Julien R., Bai, Lin, Vo, Thi, Xin, Huolin L., Li, Huilin, Li, Ruipeng, Fukuto, Masafumi, Yager, Kevin G., Kahn, Jason S., Xiong, Yan, Minevich, Brian, Kumar, Sanat K., and Gang, Oleg. Ordered three-dimensional nanomaterials using DNA-prescribed and valence-controlled material voxels. United States: N. p., 2020. Web. doi:10.1038/s41563-019-0550-x.
Tian, Ye, Lhermitte, Julien R., Bai, Lin, Vo, Thi, Xin, Huolin L., Li, Huilin, Li, Ruipeng, Fukuto, Masafumi, Yager, Kevin G., Kahn, Jason S., Xiong, Yan, Minevich, Brian, Kumar, Sanat K., & Gang, Oleg. Ordered three-dimensional nanomaterials using DNA-prescribed and valence-controlled material voxels. United States. doi:https://doi.org/10.1038/s41563-019-0550-x
Tian, Ye, Lhermitte, Julien R., Bai, Lin, Vo, Thi, Xin, Huolin L., Li, Huilin, Li, Ruipeng, Fukuto, Masafumi, Yager, Kevin G., Kahn, Jason S., Xiong, Yan, Minevich, Brian, Kumar, Sanat K., and Gang, Oleg. Mon . "Ordered three-dimensional nanomaterials using DNA-prescribed and valence-controlled material voxels". United States. doi:https://doi.org/10.1038/s41563-019-0550-x. https://www.osti.gov/servlets/purl/1600469.
@article{osti_1600469,
title = {Ordered three-dimensional nanomaterials using DNA-prescribed and valence-controlled material voxels},
author = {Tian, Ye and Lhermitte, Julien R. and Bai, Lin and Vo, Thi and Xin, Huolin L. and Li, Huilin and Li, Ruipeng and Fukuto, Masafumi and Yager, Kevin G. and Kahn, Jason S. and Xiong, Yan and Minevich, Brian and Kumar, Sanat K. and Gang, Oleg},
abstractNote = {The ability to organize nanoscale objects into well-defined three-dimensional (3D) arrays can translate advances in nanoscale synthesis into targeted material fabrication. Despite successes in nanoparticle assembly, most extant methods are system specific and not fully compatible with biomolecules. As such, here, we report a platform for creating distinct 3D ordered arrays from different nanomaterials using DNA-prescribed and valence-controlled material voxels. These material voxels consist of 3D DNA frames that integrate nano-objects within their scaffold, thus enabling the object’s valence and coordination to be determined by the frame’s vertices, which can bind to each other through hybridization. Such DNA material voxels define the lattice symmetry through the spatially prescribed valence decoupling the 3D assembly process from the nature of the nanocomponents, such as their intrinsic properties and shapes. We show this by assembling metallic and semiconductor nanoparticles and also protein superlattices. We support the technological potential of such an assembly approach by fabricating light-emitting 3D arrays with diffraction-limited spectral purity and 3D enzymatic arrays with increased activity.},
doi = {10.1038/s41563-019-0550-x},
journal = {Nature Materials},
number = 7,
volume = 19,
place = {United States},
year = {2020},
month = {1}
}

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