Title: Regulating phase behavior of nanoparticle assemblies through engineering of DNA-mediated isotropic interactions

Abstract

Self-assembly of isotropically interacting particles into desired crystal structures could allow for creating designed functional materials via simple synthetic means. However, the ability to use isotropic particles to assemble different crystal types remains challenging, especially for generating low-coordinated crystal structures. Here, we demonstrate that isotropic pairwise interparticle interactions can be rationally tuned through the design of DNA shells in a range that allows transition from common, high-coordinated FCC-CuAu and BCC-CsCl lattices, to more exotic symmetries for spherical particles such as the SC-NaCl lattice and to low-coordinated crystal structures (i.e., cubic diamond, open honeycomb). The combination of computational and experimental approaches reveals such a design strategy using DNA-functionalized nanoparticles and successfully demonstrates the realization of BCC-CsCl, SC-NaCl, and a weakly ordered cubic diamond phase. The study reveals the phase behavior of isotropic nanoparticles for DNA–shell tunable interaction, which, due to the ease of synthesis is promising for the practical realization of non-close-packed lattices.

Authors:

Mao, Runfang  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-8753-2477"

Minevich, Brian  ^[2];

• Search DOE PAGES for author "Minevich, Brian"
• Search DOE PAGES for ORCID "0000-0001-5979-6646"

McKeen, Daniel  ^[2];

• Search DOE PAGES for author "McKeen, Daniel"
• Search DOE PAGES for ORCID "0000-0001-5113-2247"

Chen, Qizan ^[3]; Lu, Fang  ^[4];

• Search DOE PAGES for author "Lu, Fang"
• Search DOE PAGES for ORCID "0000-0003-3765-7615"

Gang, Oleg ^[5]; Mittal, Jeetain  ^[6]

• Search DOE PAGES for author "Mittal, Jeetain"
• Search DOE PAGES for ORCID "0000-0002-9725-6402"

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+ Show Author Affiliations

1. Department of Chemical Engineering and Materials Science, University of Minnesota–Twin Cities, Minneapolis, MN 55455
2. Department of Chemical Engineering, Columbia University, New York, NY 10027
3. Artie McFerrin Department of Chemical Engineering, Texas A&,M University, College Station, TX 77843
4. Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY 11973
5. Department of Chemical Engineering, Columbia University, New York, NY 10027, Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY 11973, Department of Applied Physics and Applied Mathematics, Columbia University, New York, NY 10027
6. Artie McFerrin Department of Chemical Engineering, Texas A&,M University, College Station, TX 77843, Department of Chemistry, Texas A&,M University, College Station, TX 77843, Interdisciplinary Graduate Program in Genetics and Genomics, Texas A&,M University, College Station, TX 77843

Publication Date:

Mon Dec 18 00:00:00 EST 2023

Research Org.:

Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Org.:

USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF)

OSTI Identifier:

2242531

Alternate Identifier(s):

OSTI ID: 2338122

Report Number(s):

BNL-225492-2024-JAAM
Journal ID: ISSN 0027-8424; e2302037120

Grant/Contract Number:  

SC0008772; SC0012704; AC02-05CH11231; CBET 1953245; A-2113-20220331; TG-MCB120014

Resource Type:

Published Article

Journal Name:

Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:

Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 120 Journal Issue: 52; Journal ID: ISSN 0027-8424

Publisher:

Proceedings of the National Academy of Sciences

Country of Publication:

United States

Language:

English

Subject:

77 NANOSCIENCE AND NANOTECHNOLOGY; self-assembly; nanoparticles; structural DNA nanotechnology; colloidal crystallization; soft matter