ArticleProceedings of the National Academy of Sciences of the United States of America2020
Two-step crystallization and solid-solid transitions in binary colloidal mixtures.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2020. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 14 papers.
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Who cites it
14 citing papers in PubMed.
- Dual-symmetry-guided assembly of complex lattices.Nature · 2026Article
- Article
- Kinetic pathways of solid-solid phase transitions dictated by short-range interactions.Proceedings of the National Academy of Sciences of the United States of America · 2025Article
- Direct observation and control of non-classical crystallization pathways in binary colloidal systems.Nature communications · 2025Article
- Dynamic and asymmetric colloidal molecules.Nature communications · 2025Article
- Programming patchy particles for materials assembly design.Proceedings of the National Academy of Sciences of the United States of America · 2024Article
- Autonomous assembly and disassembly of gliding molecular robots regulated by a DNA-based molecular controller.Science advances · 2024Article
- In situ observation of coalescence of nuclei in colloidal crystal-crystal transitions.Nature communications · 2023Article
- Macroscopic photonic single crystals via seeded growth of DNA-coated colloids.Nature communications · 2023Article
- Geometrically programmed self-limited assembly of tubules using DNA origami colloids.Proceedings of the National Academy of Sciences of the United States of America · 2022Article
- Polymorphic self-assembly of helical tubules is kinetically controlled.Soft matter · 2022Article
- Two-dimensional binary colloidal crystals formed by particles with two different sizes.Scientific reports · 2022Article
- Comprehensive view of microscopic interactions between DNA-coated colloids.Nature communications · 2022Article
- Self-assembly of photonic crystals by controlling the nucleation and growth of DNA-coated colloids.Proceedings of the National Academy of Sciences of the United States of America · 2022Article
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Authors and funding
3 authors.
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Abstract
Crystallization is fundamental to materials science and is central to a variety of applications, ranging from the fabrication of silicon wafers for microelectronics to the determination of protein structures. The basic picture is that a crystal nucleates from a homogeneous fluid by a spontaneous fluctuation that kicks the system over a single free-energy barrier. However, it is becoming apparent that nucleation is often more complicated than this simple picture and, instead, can proceed via multiple transformations of metastable structures along the pathway to the thermodynamic minimum. In this article, we observe, characterize, and model crystallization pathways using DNA-coated colloids. We use optical microscopy to investigate the crystallization of a binary colloidal mixture with single-particle resolution. We observe classical one-step pathways and nonclassical two-step pathways that proceed via a solid-solid transformation of a crystal intermediate. We also use enhanced sampling to compute the free-energy landscapes corresponding to our experiments and show that both one- and two-step pathways are driven by thermodynamics alone. Specifically, the two-step solid-solid transition is governed by a competition between two different crystal phases with free energies that depend on the crystal size. These results extend our understanding of available pathways to crystallization, by showing that size-dependent thermodynamic forces can produce pathways with multiple crystal phases that interconvert without free-energy barriers and could provide approaches to controlling the self-assembly of materials made from colloids.
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