Crystal Nucleation in Supercooled Atomic Liquids.

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.

Refractive Index of Supercooled Water Down to 230.3 K in the Wavelength Range between 534 and 675 nm.

Knowledge of the refractive index of water in the deeply supercooled metastable liquid state is important, for example, for an accurate description of optical reflection and refraction processes occurring in clouds. However, a measurement of both the temperature and wavelength dependence of the refractive index under such extreme conditions is challenging. Here, we employ Raman spectroscopy in combination with microscopic water jets in vacuum to obtain the refractive index of supercooled water to a lowest temperature of 230.3 K. While our approach is based on the analysis of Mie resonances in Raman spectra measured by using a single excitation wavelength at 532 nm, it allows us to obtain the refractive index in a wide visible wavelength range from 534 to 675 nm. Because of a direct link between the refractive index and density of water, our results provide a promising approach to help improve our understanding of water's anomalous behavior.