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Significance Crystallization—the spontaneous formation of an ordered solid from a disordered fluid—has fascinated humankind for centuries. Contrary to longstanding theories, which predict that crystals form by a single nucleation event, recent experiments have shown that crystallization can traverse multiple intermediate states. In this paper, we observe a two-step crystallization pathway, in which a metastable crystal forms first and later transforms into another crystal with a different crystallographic symmetry. This transformation is diffusionless: The particles undergo coherent, local rearrangements. Using complementary computer simulations, we show that the two-step crystallization pathway is driven by competing thermodynamic forces and, thus, could be common to many physical systems.

Two-step crystallization and solid–solid transitions in binary colloidal mixtures