Experimental observation of the liquid-liquid transition in bulk supercooled water under pressure

Kim, Kyung Hwan; Amann‐Winkel, Katrin; Giovambattista, Nicolás; Späh, Alexander; Perakis, Fivos; Pathak, Harshad; Ladd-Parada, Marjorie; Yang, Cheolhee; Mariedahl, Daniel; Eklund, Tobias; Lane, Thomas J; You, Seonju; Jeong, Sangmin; Weston, Matthew; Lee, Jae Hyuk; Eom, Intae; Kim, Minseok; Park, Jaeku; Chun, Sae Hwan; Poole, Peter H.; Nilsson, Anders

doi:10.1126/science.abb9385

Cited by 187 publications

(229 citation statements)

References 78 publications

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“…These observations let to the conclusion that the HDA-LDA transition is actually taking place via high-and low-density liquid forms of water named HDL and LDL, i.e., a HDA-HDL-LDL-LDA transition was observed. This study provided one of the first experimental evidence for the existence of two forms of liquid water, that has been strengthened in subsequent FEL studies on water [111][112][113].…”

Section: Dynamical Heterogeneities Via Two-times Correlationsmentioning

confidence: 60%

From Femtoseconds to Hours—Measuring Dynamics over 18 Orders of Magnitude with Coherent X-rays

2021

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X-ray photon correlation spectroscopy (XPCS) enables the study of sample dynamics between micrometer and atomic length scales. As a coherent scattering technique, it benefits from the increased brilliance of the next-generation synchrotron radiation and Free-Electron Laser (FEL) sources. In this article, we will introduce the XPCS concepts and review the latest developments of XPCS with special attention on the extension of accessible time scales to sub-μs and the application of XPCS at FELs. Furthermore, we will discuss future opportunities of XPCS and the related technique X-ray speckle visibility spectroscopy (XSVS) at new X-ray sources. Due to its particular signal-to-noise ratio, the time scales accessible by XPCS scale with the square of the coherent flux, allowing to dramatically extend its applications. This will soon enable studies over more than 18 orders of magnitude in time by XPCS and XSVS.

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Section: Dynamical Heterogeneities Via Two-times Correlationsmentioning

confidence: 60%

From Femtoseconds to Hours—Measuring Dynamics over 18 Orders of Magnitude with Coherent X-rays

2021

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“…Even the last remaining link, the direct observation of the liquid-to-liquid transition above the glass transition temperature, seems to have been found: Winkel et al suggested that they observed a first-order transition between two ultraviscous liquids slightly above the two glass transition temperatures of LDA and HDA through decompression at 140 K (14). Very recently, Kim et al found evidence for a liquid-to-liquid transition by ultrafast heating of HDA to about 205 K (i.e., far above the glass transition), where bulk water rapidly crystallizes (60). At about the same time, Kringle et al locate the transition from high-to low-density states in the range from 245 to 190 K, supporting the idea of a two-state model based on vacuum experiments (61).…”

Section: Discussionmentioning

confidence: 99%

Experimental evidence for glass polymorphism in vitrified water droplets

Bachler

Giebelmann

Loerting

2021

Proc. Natl. Acad. Sci. U.S.A.

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The nature of amorphous ices has been debated for more than 35 years. In essence, the question is whether they are related to ice polymorphs or to liquids. The fact that amorphous ices are traditionally prepared from crystalline ice via pressure-induced amorphization has made a clear distinction tricky. In this work, we vitrify liquid droplets through cooling at ≥106 K ⋅ s−1 and pressurize the glassy deposit. We observe a first order–like densification upon pressurization and recover a high-density glass. The two glasses resemble low- and high-density amorphous ice in terms of both structure and thermal properties. Vitrified water shows all features that have been reported for amorphous ices made from crystalline ice. The only difference is that the hyperquenched and pressurized deposit shows slightly different crystallization kinetics to ice I upon heating at ambient pressure. This implies a thermodynamically continuous connection of amorphous ices with liquids, not crystals.

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“…It also explains, naturally, the complex behavior of water in the glass state [8,9,[24][25][26][27][28][29][30][31][32][33][34] which, arguably, is not clearly explained by other approaches, such as the singularity free scenario [35].…”

Section: Introductionmentioning

confidence: 99%

“…Although many theoretical approaches have been proposed to explain water anomalous behavior, the so-called liquid-liquid phase transition (LLPT) scenario [7,8] is currently the explanation best-supported by experiments [5,[9][10][11][12][13], computer simulations [7,[14][15][16][17][18], and theory [14,[19][20][21][22][23]. In the LLPT scenario, water at low temperatures exists in two distinct liquid states, low-density and high-density liquid (LDL and HDL).…”

Section: Introductionmentioning

confidence: 99%

“…Unfortunately, due to water rapid crystallization at these conditions, the existence of the LLCP in water has not been confirmed in experiments. Strong evidence for the existence of a LLPT in water is available from recent sub-microsecond experiments at T ≈ 205 K [9]; additional evidence of the LLPT in water is available from experiments performed at T ≈ 130 − 140 K, in the the so-called ultraviscous liquid state of water [36,37]. Many computer simulations validate the LLPT hypothesis.…”

Section: Introductionmentioning

confidence: 99%

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Liquid-Liquid Phase Transition in Supercooled H2O and D2O: A Path-Integral Computer Simulation Study

Eltareb

López

Giovambattista

2021

Preprint

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We perform path-integral molecular dynamics (PIMD) and classical MD simulations of H2O and D2O using the q-TIP4P/F water model over a wide range of temperatures and pressures. The density ρ(T), isothermal compressibility κT(T), and self-diffusion coefficients D(T) of H2O and D2O are in excellent agreement with available experimental data; the isobaric heat capacity CP(T) obtained from PIMD and MD simulations agree qualitatively well with the experiments. Some of these thermodynamic properties exhibit anomalous maxima upon isobaric cooling, consistent with recent experiments and with the possibility that H2O and D2O exhibit a liquid-liquid critical point (LLCP) at low temperatures and positive pressures. The data from PIMD/MD for H2O and D2O can be fitted remarkably well using the Two-State-Equation-of-State (TSEOS). Using the TSEOS, we estimate that the LLCP for q-TIP4P/F H2O, from PIMD simulations, is located at Pc = 167±9 MPa, Tc = 159±6 K, and ρc = 1.02±0.01 g/cm3. Isotope substitution effects are important; the LLCP location in q-TIP4P/F D2O is estimated to be Pc = 176 ± 4 MPa, Tc = 177 ± 2 K, and ρc = 1.13±0.01 g/cm3. Interestingly, for the water model studied, differences in the LLCP location from PIMD and MD simulations suggest that nuclear quantum effects (i.e., atoms delocalization) play an important role in the thermodynamics of water around the LLCP (from the MD simulations of q-TIP4P/F water, Pc = 203 ± 4 MPa, Tc = 175 ± 2 K, and ρc = 1.03 ± 0.01 g/cm3). Overall, our results strongly support the LLPT scenario to explain water anomalous behavior, independently of the fundamental differences between classical MD and PIMD techniques. The reported values of Tc for D2O and, particularly, H2O suggest that improved water models are needed for the study of supercooled water.

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Experimental observation of the liquid-liquid transition in bulk supercooled water under pressure

Cited by 187 publications

References 78 publications

From Femtoseconds to Hours—Measuring Dynamics over 18 Orders of Magnitude with Coherent X-rays

From Femtoseconds to Hours—Measuring Dynamics over 18 Orders of Magnitude with Coherent X-rays

Experimental evidence for glass polymorphism in vitrified water droplets

Liquid-Liquid Phase Transition in Supercooled H2O and D2O: A Path-Integral Computer Simulation Study

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