Many structural materials (metal alloys, polymers, minerals, etc.) are formed by quenching liquids into crystalline solids. This highly non-equilibrium process often leads to polycrystalline growth patterns that are broadly termed 'spherulites' because of their large-scale average spherical shape. Despite the prevalence and practical importance of spherulite formation, only rather qualitative concepts of this phenomenon exist. The present work explains the growth and form of these fundamental condensed matter structures on the basis of a unified field theoretic approach. Our phase field model is the first to incorporate the essential ingredients for this type crystal growth: anisotropies in both the surface energy and interface mobilities that are responsible for needle-like growth, trapping of local orientational order due to either static heterogeneities (impurities) or dynamic heterogeneities in highly supercooled liquids, and a preferred relative grain orientation induced by a misorientation-dependent grain boundary energy. Our calculations indicate that the diversity of spherulite growth forms arises from a competition between the ordering effect of discrete local crystallographic symmetries and the randomization of the local crystallographic orientation that accompanies crystal grain nucleation at the growth front (growth front nucleation or GFN). The large-scale isotropy of spherulitic growth arises from the predominance of GFN.

Here, we review the basic concepts and applications of the phase-field-crystal (PFC) method, which is one of the latest simulation methodologies in materials science for problems, where atomic-and microscales are tightly coupled. The PFC method operates on atomic length and diffusive time scales, and thus constitutes a computationally efficient alternative to molecular simulation methods. Its intense development in materials science started fairly recently following the work by Elder et al. [Phys. Rev. Lett. 88 (2002), p. 245701]. Since these initial studies, dynamical density functional theory and thermodynamic concepts have been linked to the PFC approach to serve as further theoretical fundaments for the latter. In this review, we summarize these methodological development steps as well as the most important applications of the PFC method with a special focus on the interaction of development steps taken in hard and soft matter physics, respectively. Doing so, we hope to present today's state of the art in PFC modelling as well as the potential, which might still arise from this method in physics and materials science in the nearby future.Keywords: phase-field-crystal (PFC) models, static and dynamical density functional theory (DFT and DDFT), condensed matter dynamics of liquid crystals and polymers, nucleation and pattern formation, simulations in materials science, colloidal crystal growth and growth anisotropy * Corresponding authors. Emails: heike.emmerich@uni-bayreuth. de, hlowen@thphy.uni-duesseldorf.de, and grana@szfki.hu

We apply a simple dynamical density functional theory, the phase-field crystal (PFC) model of overdamped conservative dynamics, to address polymorphism, crystal nucleation, and crystal growth in the diffusion-controlled limit. We refine the phase diagram for 3D, and determine the line free energy in 2D and the height of the nucleation barrier in 2D and 3D for homogeneous and heterogeneous nucleation by solving the respective Euler-Lagrange (EL) equations. We demonstrate that, in the PFC model, the body-centered cubic (bcc), the face-centered cubic (fcc), and the hexagonal close-packed structures (hcp) compete, while the simple cubic structure is unstable, and that phase preference can be tuned by changing the model parameters: close to the critical point the bcc structure is stable, while far from the critical point the fcc prevails, with an hcp stability domain in between. We note that with increasing distance from the critical point the equilibrium shapes vary from the sphere to specific faceted shapes: rhombic dodecahedron (bcc), truncated octahedron (fcc), and hexagonal prism (hcp). Solving the equation of motion of the PFC model supplied with conserved noise, solidification starts with the nucleation of an amorphous precursor phase, into which the stable crystalline phase nucleates. The growth rate is found to be time dependent and anisotropic; this anisotropy depends on the driving force. We show that due to the diffusion-controlled growth mechanism, which is especially relevant for crystal aggregation in colloidal systems, dendritic growth structures evolve in large-scale isothermal single-component PFC simulations. An oscillatory effective pair potential resembling those for model glass formers has been evaluated from structural data of the amorphous phase obtained by instantaneous quenching. Finally, we present results for eutectic solidification in a binary PFC model.

We use a simple density functional approach on a diffusional time scale, to address freezing to the body-centered cubic (bcc), hexagonal close-packed (hcp), and face-centered cubic (fcc) structures. We observe faceted equilibrium shapes and diffusion-controlled layerwise crystal growth consistent with twodimensional nucleation. The predicted growth anisotropies are discussed in relation with results from experiment and atomistic simulations. We also demonstrate that varying the lattice constant of a simple cubic substrate, one can tune the epitaxially growing body-centered tetragonal structure between bcc and fcc, and observe a Mullins-Sekerka-Asaro-Tiller-Grinfeld-type instability.