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Non-classical crystallization in soft and organic materials

Nature Reviews Materials volume 9, pages 229–248 (2024)Cite this article

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Abstract

Classical nucleation and crystal growth theories describe how nuclei form, become stable after reaching a critical size and then enlarge through monomer attachment. More than two decades ago, non-classical pathways have been proposed for various types of (bio)molecules and materials, which can substantially alter the crystallization kinetics and outcomes. Direct observation of non-classical crystallization of inorganic nanomaterials, including metastable structure-mediated and particle attachment-based pathways that usually occur on the nanoscale, was enabled by in situ liquid-phase electron microscopy. However, it was not until recently that the crystallization dynamics of beam-sensitive soft materials were directly imaged with sufficient spatial resolution, and a level of microstructural understanding of defects and interfaces emerged. This article provides a high-level review of the non-classical crystallization pathways discovered in soft and organic materials and a forward-looking guide for future research. We first analyse how the characteristics of soft materials affect their crystallization pathways and kinetics. We then identify technical approaches to studying the crystallization trajectories of soft materials and discuss strategies to properly select and apply them to different systems. Breakthroughs made in understanding the crystallization of small organic molecules, (bio)macromolecules, colloids and reticular framework materials are examined. Finally, we provide an outlook on the challenges in elucidating soft material crystallization pathways and the opportunities for assisting the design and synthesis of new materials and structures.

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Fig. 1: Types and thermodynamics of non-classical nucleation and crystal growth.
Fig. 2: Methods for studying the crystallization pathways of soft and organic materials.
Fig. 3: Crystallization of small organic molecules through intermediate structures.
Fig. 4: Non-classical protein crystallization.
Fig. 5: Multistep assembly of polymers into ordered structures.
Fig. 6: Non-classical nucleation and growth in microscale and nanoscale colloidal crystals.
Fig. 7: Building units and their non-classical evolution in MOFs and COFs.

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Acknowledgements

The authors thank the anonymous reviewers for their constructive feedback. This work was carried out at Pacific Northwest National Laboratory (PNNL) with support from the US Department of Energy (DOE) Office of Science (SC) Basic Energy Sciences (BES) programme. Review of biomacromolecules was supported by the US DOE SC BES as part of the Energy Frontier Research Centers programme: CSSAS (The Center for the Science of Synthesis Across Scales) under Award DE-SC0019288 (FWP 72448 at PNNL). Review of reticular framework materials and small organic molecules was supported by the US DOE SC BES Division of Materials Science and Engineering (MSE) Synthesis and Processing Sciences programme under Award FWP 67554 at PNNL. Review of colloids and techniques was supported by the US DOE SC BES MSE Biomolecular Materials programme under Award FWP 65357 at PNNL. J.S.D. acknowledges a Washington Research Foundation Postdoctoral Fellowship. Pacific Northwest National Laboratory is a multiprogramme national laboratory operated for the DOE by Battelle under Contract DE-AC05-76RL01830.

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Authors and Affiliations

  1. Physical Sciences Division, Pacific Northwest National Laboratory, Richland, WA, USA

    Jingshan S. Du, Yuna Bae & James J. De Yoreo

  2. Department of Materials Science and Engineering, University of Washington, Seattle, WA, USA

    James J. De Yoreo

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Contributions

J.S.D. and J.J.D.Y. conceived and defined the scope of this Review. J.S.D. drafted the introduction, the section ‘Technique selection for studying crystallization pathways’, the subsection ‘Organic molecular crystals’, the section ‘Non-classical crystallization in reticular framework materials’ and the section ‘Outlook’. Y.B. drafted the sections ‘Macromolecular crystals’ and ‘Colloidal crystals’. All authors discussed and edited the manuscript.

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Correspondence to James J. De Yoreo.

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Du, J.S., Bae, Y. & De Yoreo, J.J. Non-classical crystallization in soft and organic materials. Nat Rev Mater 9, 229–248 (2024). https://doi.org/10.1038/s41578-023-00637-y

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