title: Growth rate of crystalline ice and the diffusivity of supercooled water from 126 to 262 K.
abstract: Understanding deeply supercooled water is key to unraveling many of water's anomalous properties. However, developing this understanding has proven difficult due to rapid and uncontrolled crystallization. Using a pulsed-laser-heating technique, we measure the growth rate of crystalline ice, G(T), for 180 K < T < 262 K, that is, deep within water's "no man's land" in ultrahigh-vacuum conditions. Isothermal measurements of G(T) are also made for 126 K ≤ T ≤ 151 K. The self-diffusion of supercooled liquid water, D(T), is obtained from G(T) using the Wilson-Frenkel model of crystal growth. For T > 237 K and P ∼ 10-8Pa, G(T) and D(T) have super-Arrhenius ("fragile") temperature dependences, but both cross over to Arrhenius ("strong") behavior with a large activation energy in no man's land. The fact that G(T) and D(T) are smoothly varying rules out the hypothesis that liquid water's properties have a singularity at or near 228 K at ambient pressures. However, the results are consistent with a previous prediction for D(T) that assumed no thermodynamic transitions occur in no man's land.
authors.affiliation: Chemical Physics & Analysis, Physical Sciences Division, Physical & Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA 99352.
authors.forename: Yuntao
authors.initials: Y
authors.lastname: Xu
authors.affiliation: Chemical Physics & Analysis, Physical Sciences Division, Physical & Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA 99352.
authors.forename: Nikolay G
authors.identifier: 0000-0001-7129-0752
authors.initials: NG
authors.lastname: Petrik
authors.affiliation: Chemical Physics & Analysis, Physical Sciences Division, Physical & Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA 99352.
authors.forename: R Scott
authors.initials: RS
authors.lastname: Smith
authors.affiliation: Chemical Physics & Analysis, Physical Sciences Division, Physical & Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA 99352 gregory.kimmel@pnnl.gov bruce.kay@pnnl.gov.
authors.forename: Bruce D
authors.initials: BD
authors.lastname: Kay
authors.affiliation: Chemical Physics & Analysis, Physical Sciences Division, Physical & Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA 99352 gregory.kimmel@pnnl.gov bruce.kay@pnnl.gov.
authors.forename: Greg A
authors.identifier: 0000-0003-4447-2440
authors.initials: GA
authors.lastname: Kimmel
keywords: crystallization kinetics; dynamic crossover; self-diffusion; supercooled water