Design and synthesis of multigrain nanocrystals via geometric misfit strain

Myoung Hwan Oh, Min Gee Cho, Dong Young Chung, Inchul Park, Youngwook Paul Kwon, Colin Ophus, Dokyoon Kim, Min Gyu Kim, Beomgyun Jeong, X. Wendy Gu, Jinwoung Jo, Ji Mun Yoo, Jaeyoung Hong, Sara McMains, Kisuk Kang, Yung-Eun Sung, A. Paul Alivisatos () and Taeghwan Hyeon ()
Additional contact information
Myoung Hwan Oh: Institute for Basic Science (IBS)
Min Gee Cho: Institute for Basic Science (IBS)
Dong Young Chung: Institute for Basic Science (IBS)
Inchul Park: Institute for Basic Science (IBS)
Youngwook Paul Kwon: University of California Berkeley
Colin Ophus: Lawrence Berkeley National Laboratory
Dokyoon Kim: Institute for Basic Science (IBS)
Min Gyu Kim: Pohang University of Science and Technology
Beomgyun Jeong: Korea Basic Science Institute
X. Wendy Gu: Department of Mechanical Engineering, Stanford University
Jinwoung Jo: Institute for Basic Science (IBS)
Ji Mun Yoo: Institute for Basic Science (IBS)
Jaeyoung Hong: Institute for Basic Science (IBS)
Sara McMains: University of California Berkeley
Kisuk Kang: Institute for Basic Science (IBS)
Yung-Eun Sung: Institute for Basic Science (IBS)
A. Paul Alivisatos: University of California Berkeley
Taeghwan Hyeon: Institute for Basic Science (IBS)

Nature, 2020, vol. 577, issue 7790, 359-363

Abstract: Abstract The impact of topological defects associated with grain boundaries (GB defects) on the electrical, optical, magnetic, mechanical and chemical properties of nanocrystalline materials1,2 is well known. However, elucidating this influence experimentally is difficult because grains typically exhibit a large range of sizes, shapes and random relative orientations3–5. Here we demonstrate that precise control of the heteroepitaxy of colloidal polyhedral nanocrystals enables ordered grain growth and can thereby produce material samples with uniform GB defects. We illustrate our approach with a multigrain nanocrystal comprising a Co3O4 nanocube core that carries a Mn3O4 shell on each facet. The individual shells are symmetry-related interconnected grains6, and the large geometric misfit between adjacent tetragonal Mn3O4 grains results in tilt boundaries at the sharp edges of the Co3O4 nanocube core that join via disclinations. We identify four design principles that govern the production of these highly ordered multigrain nanostructures. First, the shape of the substrate nanocrystal must guide the crystallographic orientation of the overgrowth phase7. Second, the size of the substrate must be smaller than the characteristic distance between the dislocations. Third, the incompatible symmetry between the overgrowth phase and the substrate increases the geometric misfit strain between the grains. Fourth, for GB formation under near-equilibrium conditions, the surface energy of the shell needs to be balanced by the increasing elastic energy through ligand passivation8–10. With these principles, we can produce a range of multigrain nanocrystals containing distinct GB defects.

Date: 2020
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DOI: 10.1038/s41586-019-1899-3

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