Liquid-liquid phase separation in supercooled water from ultrafast heating of low-density amorphous ice

Author:

Amann-Winkel KatrinORCID,Kim Kyung Hwan,Giovambattista NicolasORCID,Ladd-Parada MarjorieORCID,Späh Alexander,Perakis FivosORCID,Pathak Harshad,Yang Cheolhee,Eklund Tobias,Lane Thomas J.ORCID,You SeonjuORCID,Jeong Sangmin,Lee Jae HyukORCID,Eom IntaeORCID,Kim Minseok,Park JaekuORCID,Chun Sae HwanORCID,Poole Peter H.ORCID,Nilsson AndersORCID

Abstract

AbstractRecent 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.

Publisher

Springer Science and Business Media LLC

Subject

General Physics and Astronomy,General Biochemistry, Genetics and Molecular Biology,General Chemistry,Multidisciplinary

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