Direct observation and control of non-classical crystallization pathways in binary colloidal systems

Shihao Zang, Sanjib Paul, Cheuk W. Leung, Michael S. Chen, Theodore Hueckel, Glen M. Hocky () and Stefano Sacanna ()
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Shihao Zang: New York University
Sanjib Paul: New York University
Cheuk W. Leung: New York University
Michael S. Chen: New York University
Theodore Hueckel: New York University
Glen M. Hocky: New York University
Stefano Sacanna: New York University

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: Abstract Crystallization stands as a prime example of self-assembly. Elementary building blocks converge, seemingly adhering to an intricate blueprint, orchestrating order from chaos. While classical theories describe crystallization as a monomer-by-monomer addition, non-classical pathways introduce complexity. Using microscopic charged particles as monomers, we uncover the mechanisms governing the formation of ionic colloidal crystals. Our findings reveal a two-step process, wherein metastable amorphous blobs condense from the gas phase, before evolving into small binary crystals. These small crystals then grow into large faceted structures via three simultaneous processes: addition of free monomers from bulk, capture and absorption of surrounding blobs, and oriented attachment of other crystals. These complex crystallization pathways occur both in bulk and on surfaces across a range of particle sizes and interaction strengths, resulting in a diverse array of crystal types and morphologies. Harnessing our ability to tune the interaction potential through small changes in salt concentration, we developed a continuous dialysis approach that allows fine control over the interaction strength in both time and space. This method enables us to discover and characterize various crystal structures in a single experiment, including a previously unreported low-density hollow structure and the heteroepitaxial formation of composite crystal structures.

Date: 2025
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DOI: 10.1038/s41467-025-58959-0

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