Title: Two-Stage Assembly of Nanoparticle Superlattices with Multiscale Organization

Abstract

Self-assembly processes, while promising for enabling the fabrication of complexly organized nanomaterials from nanoparticles, are often limited in creating structures with multiscale order. These limitations are due to difficulties in practically realizing the assembly processes required to achieve such complex organizations. For a long time, a hierarchical assembly attracted interest as a potentially powerful approach. However, due to the experimental limitations, intermediate-level structures are often heterogeneous in composition and structure, which significantly impacts the formation of large-scale organizations. Here, we introduce a two-stage assembly strategy: DNA origami frames scaffold a coordination of nanoparticles into designed 3D nanoclusters, and then these clusters are assembled into ordered lattices whose types are determined by the clusters’ valence. Through modulating the nanocluster architectures and intercluster bindings, we demonstrate the successful formation of complexly organized nanoparticle crystals. To conclude, the presented two-stage assembly method provides a powerful fabrication strategy for creating nanoparticle superlattices with prescribed unit cells.

Authors:

Dong, Yuxiang ^[1]; Liu, Jiliang ^[2]; Lu, Xuanzhao  ^[1];

• Search DOE PAGES for author "Lu, Xuanzhao"
• Search DOE PAGES for ORCID "0000-0002-5991-8196"

Duan, Jialin ^[3]; Zhou, Liqi ^[1]; Dai, Lizhi ^[1]; Ji, Min ^[1]; Ma, Ningning ^[1]; Wang, Yong ^[1]; Wang, Peng  ^[4];

• Search DOE PAGES for author "Wang, Peng"
• Search DOE PAGES for ORCID "0000-0003-0788-6687"

Zhu, Jun-Jie  ^[1];

• Search DOE PAGES for author "Zhu, Jun-Jie"
• Search DOE PAGES for ORCID "0000-0002-8201-1285"

Min, Qianhao  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-7559-8743"

Gang, Oleg  ^[5];

• Search DOE PAGES for author "Gang, Oleg"
• Search DOE PAGES for ORCID "0000-0001-5534-3121"

Tian, Ye  ^[1]

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• Search DOE PAGES for ORCID "0000-0003-3137-7700"

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+ Show Author Affiliations

1. Nanjing Univ. (China)
2. European Synchrotron Radiation Facility (ESRF), Grenoble (France)
3. Chinese Academy of Sciences (CAS), Shanghai (China)
4. Nanjing Univ. (China); Univ. of Warwick, Coventry (United Kingdom)
5. Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Publication Date:

Mon Apr 25 00:00:00 EDT 2022

Research Org.:

Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); Fundamental Research Funds for the Central Universities; Shenzhen International Cooperation Research Project; China National Postdoctoral Program for Innovative Talents

OSTI Identifier:

1890435

Report Number(s):

BNL-223528-2022-JAAM
Journal ID: ISSN 1530-6984

Grant/Contract Number:  

SC0012704; SC0008772; 21834004; 92056114; 020514380255; 21971109; 11874199; GJHZ20180930090602235; BX2021119

Resource Type:

Accepted Manuscript

Journal Name:

Nano Letters

Additional Journal Information:

Journal Volume: 22; Journal Issue: 9; Journal ID: ISSN 1530-6984

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

English

Subject:

36 MATERIALS SCIENCE; DNA nanotechnology; DNA origami; self-assembly; nanoparticles; DNA nanostructures