Dynamic Transformation of High-Architectural Nanocrystal Superlattices upon Solvent Molecule Exposure

Nagaoka, Yasutaka; Schneider, Jeremy; Jin, Na; Cai, Tong; Liu, Yuzi; Wang, Zhongwu; Li, Ruipeng; Kim, Kyung-Suk; Chen, Ou

doi:10.1021/jacs.3c14603

Title: Dynamic Transformation of High-Architectural Nanocrystal Superlattices upon Solvent Molecule Exposure

Journal Article · 01 May 2024 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.3c14603 · OSTI ID:2432568

^[1];

^[1]; Jin, Na ^[1]; Cai, Tong ^[1];

^[2];

^[3]; Li, Ruipeng ^[4]; Kim, Kyung-Suk ^[1];

^[1]

Brown Univ., Providence, RI (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
Cornell Univ., Ithaca, NY (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

The cluster-based body-centered-cubic superlattice (cBCC SL) represents one of the most complicated structures among reported nanocrystal assemblies, comprised of 72 truncated tetrahedral quantum dots per unit cell. Our previous report revealed that truncated tetrahedral quantum dots within cBCC SLs possessed highly controlled translational and orientational order owing to an unusual energetic landscape based on the balancing of entropic and enthalpic contributions during the assembly process. However, the cBCC SL’s structural transformability and mechanical properties, uniquely originating from such complicated nanostructures, have yet to be investigated. Herein, we report that cBCC SLs can undergo dynamic transformation to face-centered-cubic SLs in response to post-assembly molecular exposure. We monitored the dynamic transformation process using in situ synchrotron-based small-angle X-ray scattering, revealing a dynamic transformation involving multiple steps underpinned by interactions between incoming molecules and TTQDs’ surface ligands. Furthermore, our mechanistic study demonstrated that the precise configuration of TTQDs’ ligand molecules in cBCC SLs was key to their high structural transformability and unique jelly-like soft mechanical properties. While ligand molecular configurations in nanocrystal SLs are often considered minor features, our findings emphasize their significance in controlling weak van der Waals interactions between nanocrystals within assembled SLs, leading to previously unremarked superstructural transformability and unique mechanical properties. Finally, our findings promote a facile route toward further creation of soft materials, nanorobotics, and out-of-equilibrium assemblies based on nanocrystal building blocks.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF); Alfred P. Sloan Foundation

Grant/Contract Number:: SC0012704; AC02-06CH11357

OSTI ID:: 2432568

Report Number(s):: BNL--225946-2024-JAAM

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 19 Vol. 146; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
X-ray scattering
chemical structure
ligands
molecules
solvents

Title: Dynamic Transformation of High-Architectural Nanocrystal Superlattices upon Solvent Molecule Exposure

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