Crystal Nucleation in Supercooled Atomic Liquids
Johannes Möller, Alexander Schottelius, Michele Caresana, Ulrike Boesenberg, Chan Kim, Francesco Dallari, Tiberio A. Ezquerra, J. M. Fernández, Luca Gelisio, Andrea Glaesener, Claudia Goy, Jörg Hallmann, Anton Kalinin, Ruslan P. Kurta, Dmitry Lapkin, Felix Lehmkühler, Francesco Mambretti, Markus Scholz, Roman Shayduk, Florian Trinter, Ivan Vartaniants, Alexey Zozulya, D. E. Galli, G. Grübel, Anders Madsen, Frédéric Caupin, R. E. Grisenti
Abstract
The liquid-to-solid phase transition is a complex process that is difficult to investigate experimentally with sufficient spatial and temporal resolution. A key aspect of the transition is the formation of a critical seed of the crystalline phase in a supercooled liquid, that is, a liquid in a metastable state below the melting temperature. This stochastic process is commonly described within the framework of classical nucleation theory, but accurate tests of the theory in atomic and molecular liquids are challenging. Here, we employ femtosecond x-ray diffraction from microscopic liquid jets to study crystal nucleation in supercooled liquids of the rare gases argon and krypton. Our results provide stringent limits to the validity of classical nucleation theory in atomic liquids, and offer the long-sought possibility of testing nonclassical extensions of the theory.