Abstract

Recent studies have demonstrated novel strategies for the organization of nanomaterials into three-dimensional (3D) ordered arrays with prescribed lattice symmetries using DNA-based self-assembly strategies. In one approach, the nanomaterial is sequestered into DNA origami frames or “material voxels” and then coordinated into ordered arrays based on the voxel geometry and the corresponding directional interactions based on its valency. While the lattice symmetry is defined by the valency of the bonds, a larger-scale morphological development is affected by assembly processes and differences in energies of anisotropic bonds. To facilely model this assembly process, we investigate the self-assembly behavior of hard particles with six interacting vertices via theory and Monte Carlo simulations and exploration of corresponding experimental systems. We demonstrate that assemblies with different 3D crystalline morphologies, but the same lattice symmetry can be formed depending on the relative strength of vertex-to-vertex interactions in orthogonal directions. We observed three distinct assembly morphologies for such systems: cube-like, sheet-like, and cylinder-like. A simple analytical theory inspired by well-established ideas in the areas of protein crystallization, based on calculating the second virial coefficient of patchy hard spheres, captures the simulation results and thus represents a straightforward means of modeling this self-assembly process. To complement themore » theory and simulations, experimental studies were performed to investigate the assembly of octahedral DNA origami frames with varying binding energies at their vertices. In conclusion, x-ray scattering confirms the robustness of the formed nanoscale lattices for different binding energies, while both optical and electron microscopy imaging validated the theoretical predictions on the dependence of the distinct morphologies of assembled state on the interaction strengths in the three orthogonal directions.« less

Authors:

Adhikari, Sabin  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-0184-3574"

Minevich, Brian  ^[1];

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• Search DOE PAGES for ORCID "0000-0001-5979-6646"

Redeker, Daniel  ^[1];

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• Search DOE PAGES for ORCID "0000-0001-9428-1031"

Michelson, Aaron Noam  ^[2];

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• Search DOE PAGES for ORCID "0000-0003-3060-3788"

Emamy, Hamed  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-5078-5569"

Shen, Eric ^[1]; Gang, Oleg  ^[2];

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• Search DOE PAGES for ORCID "0000-0001-5534-3121"

Kumar, Sanat K.  ^[1]

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• Search DOE PAGES for ORCID "0000-0002-6690-2221"

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+ Show Author Affiliations

1. Columbia University, New York, NY (United States)
2. Columbia University, New York, NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Publication Date:

Thu Aug 31 00:00:00 EDT 2023

Research Org.:

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

Sponsoring Org.:

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

OSTI Identifier:

2204616

Report Number(s):

BNL-224986-2023-JAAM
Journal ID: ISSN 0002-7863

Grant/Contract Number:  

SC0012704; SC0008772

Resource Type:

Accepted Manuscript

Journal Name:

Journal of the American Chemical Society

Additional Journal Information:

Journal Volume: 145; Journal Issue: 36; Journal ID: ISSN 0002-7863

Publisher:

American Chemical Society (ACS)

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; Chemical structure; Genetics; Lattices; Morphology; Self organization