title: Role of the prestructured surface cloud in crystal nucleation.
abstract: For the homogeneous crystal nucleation process in a soft-core colloid model, we identify optimal reaction coordinates from a set of novel order parameters based on the local structure within the nucleus, by employing transition path sampling techniques combined with a likelihood maximization of the committor function. We find that nucleation is governed by solid clusters that consist of an hcp core embedded within a cloud of surface particles that are highly correlated with their nearest neighbors but not ordered in a high-symmetry crystal structure. The results shed new light on the interpretation of the surface and volume terms in classical nucleation theory.
authors.affiliation: Van 't Hoff Institute for Molecular Sciences, PO Box 94157, 1090 GD Amsterdam, The Netherlands.
authors.forename: Wolfgang
authors.initials: W
authors.lastname: Lechner
authors.forename: Christoph
authors.initials: C
authors.lastname: Dellago
authors.forename: Peter G
authors.initials: PG
authors.lastname: Bolhuis
mesh_terms: D003460:Crystallization; D008958:Models, Molecular; D008968:Molecular Conformation; D011336:Probability; D013499:Surface Properties