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<p>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.</p>

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

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年4月17日

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  • Shihao Zang,
  • Sanjib Paul,
  • Cheuk W. Leung,
  • Michael S. Chen,
  • Theodore Hueckel,
  • Glen M. Hocky,
  • Stefano Sacanna

摘要

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.