Driving forces for particle-based crystallization: From experiments to theory and simulations

The multistep crystallization processes involving the formation of stable building blocks that subsequently assemble into a crystal are ubiquitous in mineral formation and biomineralization and are particularly attractive in materials synthesis. Utilizing these pathways offers the approach to overcoming the restrictions on the expression of various crystal faces imposed by the interfacial energy during monomer-by-monomer growth to unlock the breadth of architectures with unique properties. Controlling particle-based crystallization proved challenging despite its promise due to the complex interdependence of interfacial forces and their nonlinear dependence on synthesis parameters. Here, the status of the development of state-of-the-art approaches to measuring interparticle forces and predictive theoretical models of particle-based crystallization are reviewed.