Mesocrystal growth through oriented sliding and attachment of nanoplates

Li, Xiaoxu; Ho, Tuan A.; Zhang, Honghu; Liu, Lili; Li, Ruipeng; Chen, Ping; Bowden, Mark E.; Mergelsberg, Sebastian T.; Fan, Hongyou; De Yoreo, James J.; Pearce, Carolyn I.; Rosso, Kevin M.; Zhang, Xin

doi:10.1038/s41467-025-64852-7

Mesocrystal growth through oriented sliding and attachment of nanoplates

Journal Article · Mon Dec 15 00:00:00 EST 2025 · Nature Communications

DOI:https://doi.org/10.1038/s41467-025-64852-7· OSTI ID:3010972

^[1]; Ho, Tuan A. ^[2]; ^[3]; ^[1]; ^[3]; Chen, Ping ^[1]; ^[1]; ^[1]; ^[2]; ^[1]; ^[1]; ^[1]; ^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Oriented attachment is a critical, yet poorly understood, crystal growth pathway based on the self-assembly of nanocrystals. During oriented attachment, solvent-separated particles align and coalesce through forces that enable precise rotation and translation. While prior studies emphasized intragap forces driving crystallographic alignment, the forces enabling uniform stacking and superlattice formation remain unclear. Here, we demonstrate how macroscopic gibbsite mesocrystals emerge from nanoplates guided into staggered positions by directional sliding. Electron microscopy and X-ray scattering reveal the monoclinic superlattice structure, based on nanoplate stacking with a uniform ≈50° stagger along the gibbsite [010] direction. In situ liquid-cell TEM captures preferential sliding along the gibbsite [010] direction, decelerating with increasing particle overlap. Molecular dynamics simulations reveal that this staggered arrangement corresponds to a global free-energy minimum, rather than full alignment. The simulations also confirm that sliding along the [010] direction is energetically favored and provide insight into the role of interfacial water in achieving long-range ordered assemblies. These insights highlight the energy landscape’s role in oriented attachment, with implications for material synthesis and hierarchical structures in nature.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830; NA0003525; SC0012704

Other Award/Contract Number:: FWP68932
FWP56674
FWP24-015452

OSTI ID:: 3010972

Alternate ID(s):: OSTI ID: 3028505

Report Number(s):: BNL--229284-2025-JAAM; PNNL-SA-207975

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 16; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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