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

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.

Liquid–Liquid Criticality in TIP4P/2005 and Three-State Models of Water

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“…This coexistence line between the two competing liquids is connected to a first-order phase transition between two glassy phases at even lower temperatures. [88][89][90][91][92][93][94][95] The presence of a density anomaly, characterized by a maximum in density upon heating along an isobar, is a wellknown and fundamental anomaly in water. In Fig.…”

Calibrating TDDFT Calculations of the X-ray Emission Spectrum of Liquid Water: The Effects of Hartree–Fock Exchange

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