Liquid-liquid phase separation in supercooled water from ultrafast heating of low-density amorphous ice
Katrin Amann‐Winkel, Kyung Hwan Kim, Nicolás Giovambattista, Marjorie Ladd-Parada, Alexander Späh, Fivos Perakis, Harshad Pathak, Cheolhee Yang, Tobias Eklund, Thomas J. Lane, Seonju You, Sangmin Jeong, Jae Hyuk Lee, Intae Eom, Minseok Kim, Jaeku Park, Sae Hwan Chun, Peter H. Poole, Anders Nilsson
Abstract
Recent experiments continue to find evidence for a liquid-liquid phase transition (LLPT) in supercooled water, which would unify our understanding of the anomalous properties of liquid water and amorphous ice. These experiments are challenging because the proposed LLPT occurs under extreme metastable conditions where the liquid freezes to a crystal on a very short time scale. Here, we analyze models for the LLPT to show that coexistence of distinct high-density and low-density liquid phases may be observed by subjecting low-density amorphous (LDA) ice to ultrafast heating. We then describe experiments in which we heat LDA ice to near the predicted critical point of the LLPT by an ultrafast infrared laser pulse, following which we measure the structure factor using femtosecond x-ray laser pulses. Consistent with our predictions, we observe a LLPT occurring on a time scale < 100 ns and widely separated from ice formation, which begins at times >1 μs.