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We have only rules of thumb with which to predict how a material willcrystallize, chief among which is Ostwald's rule of stages. It states that thefirst phase to appear upon transformation of a parent phase is the one closestto it in free energy. Although sometimes upheld, the rule is withouttheoretical foundation and is not universally obeyed, highlighting the need formicroscopic understanding of crystallization controls. Here we study in detailthe crystallization pathways of a prototypical model of patchy particles. Therange of crystallization pathways it exhibits is richer than can be predictedby Ostwald's rule, but a combination of simulation and analytic theory revealsclearly how these pathways are selected by microscopic parameters. Our resultssuggest strategies for controlling self-assembly pathways in simulation andexperiment.

Limit of validity of Ostwald's rule of stages in a statistical mechanical model of crystallization