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  • Open Access

Evolution of Polycrystallinity in Homogeneously Nucleated Colloidal Crystals

Merin Jose1, Nicholas H. P. Orr2, Taiki Yanagishima3,4,*, and Roel P. A. Dullens1,†

  • *Contact author: yanagishima-taiki@tmu.ac.jp
  • †Contact author: roel.dullens@ru.nl
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Phys. Rev. X 16, 031036 – Published 12 August, 2026

DOI: https://doi.org/10.1103/ht63-96gl

Abstract

We investigate how polycrystallinity evolves in homogeneously nucleated crystals in an experimental hard-sphere-like colloidal system using three-dimensional confocal microscopy. We capture the whole process of nucleation and crystal growth and use a recently developed method to resolve grain structure and misorientation between adjacent grains and nearest-neighbor clusters. Closely following nucleation, crystals are shown to give rise to grains through the emergence of stacking faults and twinning. The birth rate of new grains from a single nucleation event are measured, observed to increase, and then plateau. We visualize the spatial structure of a nucleus which comprises a highly ordered core and a radial increase in misorientation angles. Finally, we use local misorientation to formulate a measure for positional order which reveals a sharp decoupling between the development of orientational order and positional order at times significantly after nucleation.

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Popular Summary

Most crystalline materials consist of many differently orientated crystallites called grains. However, the role that grain formation plays during the birth and growth of polycrystalline materials is largely unknown. We used particle-resolved confocal microscopy and a recently developed analysis method to study colloidal crystallization, distinguishing and quantifying the orientation difference between neighboring clusters of particles as crystals are born and grow. We were able to distinguish individual grains as they are formed and measure the rate at which grains are spontaneously created. This has been difficult to accomplish experimentally, despite being a key ingredient for theoretical models. We also developed a metric for positional order, which shows that the orientations of adjacent unit cells align themselves significantly before “positional” order develops during growth. Observations in colloids translate to more complex crystals like metals and alloys, where grain structure can be tuned to directly impact physical properties like hardness, ductility, and malleability.

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Phys. Rev. X 16, 031036– Published 12 August, 2026
  • Received 7 January 2026
  • Accepted 29 June 2026
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.

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