Erratum: “Two-structure thermodynamics for the TIP4P/2005 model of water covering supercooled and deeply stretched regions” [J. Chem. Phys. 146, 034502 (2017)]

Biddle, John; Singh, Rakesh S.; Sparano, Evan M.; Ricci, Francesco; González, Miguel A.; Valeriani, Chantal; Abascal, J. L. F.; Debenedetti, Pablo G.; Анисимов, М. А.; Caupin, Frédéric

doi:10.1063/1.5024509

Cited by 10 publications

(18 citation statements)

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“…A two-state picture of water leading to predominance at ambient conditions of close-packing of molecules (HDL, favored by entropy), but with local fluctuations into tetrahedral environments (LDL, favored by enthalpy) is fully consistent with thermodynamics, where such models have been shown to quantitatively reproduce the thermodynamic properties of water over a wide range of temperatures and pressures 21,24,36,37 . Polarization-dependent vibrational Raman spectroscopy at the OH-stretch in H2O has concluded a 3:1 ratio at ambient conditions between molecules in disordered versus symmetric tetrahedral local environment 38 ; this is consistent with XAS and XES 6, 9-11 .…”

Section: Introductionmentioning

confidence: 78%

Relationship between x-ray emission and absorption spectroscopy and the local H-bond environment in water

Zhovtobriukh

Besley

Fransson

et al. 2018

The Journal of Chemical Physics

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The connection between specific features in the water X-ray absorption spectrum and X-ray emission spectrum (XES) and the local H-bond coordination is studied based on structures obtained from path-integral molecular dynamics simulations using either the opt-PBE-vdW density functional or the MB-pol force field. Computing the XES spectrum using all molecules in a snapshot results in only one peak in the lone-pair (1b) region, while the experiment shows two peaks separated by 0.8-0.9 eV. Different H-bond configurations were classified based on the local structure index (LSI) and a geometrical H-bond cone criterion. We find that tetrahedrally coordinated molecules characterized by high LSI values and two strong donated and two strong accepted H-bonds contribute to the low energy 1b emission peak and to the post-edge region in absorption. Molecules with the asymmetric H-bond environment with one strong accepted H-bond and one strong donated H-bond and low LSI values give rise to the high energy 1b peak in the emission spectrum and mainly contribute to the pre-edge and main-edge in the absorption spectrum. The 1b peak splitting can be increased to 0.62 eV by imposing constraints on the H-bond length, i.e., for very tetrahedral structures short H-bonds (less than 2.68 Å) and for very asymmetric structures elongated H-bonds (longer than 2.8 Å). Such structures are present, but underrepresented, in the simulations which give more of an average of the two extremes.

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Section: Introductionmentioning

confidence: 78%

Relationship between x-ray emission and absorption spectroscopy and the local H-bond environment in water

Zhovtobriukh

Besley

Fransson

et al. 2018

The Journal of Chemical Physics

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“…The properties we have found, together with previous results (2,3), thus constitute a general framework to describe and understand the anomalies of other liquids presenting a density maximum. (17). The liquid-liquid transition (solid black line) ending at a liquid-liquid critical point (C 2 ), and the spinodal line (dashed gray line) for this model are also shown.…”

mentioning

confidence: 99%

“…They can be used to locate the lines of extrema in thermodynamic functions, in order to compare them with our experimental and theoretical findings. Recently, simulations of the TIP4P/2005 potential for water have been parameterized down to the liquid-vapor spinodal with a two-state model that provides analytic formulas for all thermodynamic properties (17). The model reproduces well the lines of ex-trema that were directly simulated for TIP4P/2005, and allow to compute other lines such as LMc|P or Lmc|P .…”

mentioning

confidence: 99%

Compressibility Anomalies in Stretched Water and Their Interplay with Density Anomalies

Holten

Qiu

Guillerm

et al. 2017

J. Phys. Chem. Lett.

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Water keeps puzzling scientists because of its numerous properties which behave oppositely to usual liquids: for instance, water expands upon cooling, and liquid water is denser than ice. To explain this anomalous behaviour, several theories have been proposed, with different predictions for the properties of supercooled water (liquid at conditions where ice is more stable). However, discriminating between those theories with experiments has remained elusive because of spontaneous ice nucleation. Here we measure the sound velocity in liquid water stretched to negative pressure, and derive an experimental equation of state, which reveals compressibility anomalies. We show by rigorous thermodynamic relations how these anomalies are intricately linked with the density anomaly. Some features we observe are necessary conditions for the validity of two theories of water.Liquid water exhibits numerous anomalies and different scenarios have been proposed to explain them (1). In particular, the existence of a line of density maxima along isobars has been related to putative maxima in compressibility (2) and heat capacity (3). These maxima may arise from an intriguing phase separation of water in two distinct liquids (1,4), although they can also be explained without resorting to such a phase separation (2). However, the compressibility and heat capacity maxima, whose existence is predicted by molecular dynamics simulations (3,5), have hitherto not been observed in experiments. Alternative theoretical scenarios, namely 1 arXiv:1708.00063v1 [physics.chem-ph] 31 Jul 2017 the stability limit conjecture (6) and the critical-point-free scenario (7, 8), do not require the existence of compressibility and heat capacity maxima, but rather predict a divergence of these quantities at low temperature.Another type of anomaly, namely a minimum in sound velocity along one isochore, was recently discovered at negative pressure (9,10). At negative pressure, the liquid is mechanically stretched, in a state metastable with respect to vapor. To date, the only method able to reach significantly negative pressures (beyond −100 MPa) uses 3 − 10 µm fluid inclusions (FIs) of water in a quartz crystal, and stretching is obtained by cooling liquid water at nearly constant volume (11,12). In our previous work (9, 10), we could only study two FIs along different isochores, and only one clearly showed a minimum in sound velocity. In the present work, we have measured more FIs showing a sound velocity minimum, and reached more negative pressures. We have thus established a more accurate experimental equation of state (EoS) down to −137 MPa. The new EoS strongly supports the existence of the compressibility maxima predicted by some theories of water. Furthermore, we establish new thermodynamic relations between the line of density maxima and the sound velocity anomalies. In contrast to previous works, this provides a relation between quantities that are directly observable in experiments. The corresponding lines of extrema obtained from our experimenta...

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“…Whether TIP4P/2005, 51 one of the most accurate water models, 52 exhibits an LLCP or not is currently under debate. [53][54][55][56][57][58][59][60][61] Most computational studies (including the ones listed in Table 1) are consistent with the existence of an LLCP in TIP4P/2005. However, in the case of some water models such as SPC/E and mW, an LLCP/LLPT is not accessible.…”

Section: Liquid Water: Anomalous Properties and The Liquid-liquid Phamentioning

confidence: 62%

“…For example, a recent equation of state for TIP4P/2005 water has been obtained using a two-state water model. 54,58 This equation of state indicates that the LLCP should be located at T c = 182 K, p c = 170 MPa, and r c = 1.017 g cm À3 . Similarly, an equation of state for TIP4P/2005 water based on the potential energy landscape approach predicts that T c = 175 K, p c = 175 MPa, and r c = 0.997 g cm À3 .…”

Section: Other Salt Solutionsmentioning

confidence: 99%

Glass polymorphism and liquid–liquid phase transition in aqueous solutions: experiments and computer simulations

Bachler

Handle

Giovambattista

et al. 2019

Phys. Chem. Chem. Phys.

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Erratum: “Two-structure thermodynamics for the TIP4P/2005 model of water covering supercooled and deeply stretched regions” [J. Chem. Phys. 146, 034502 (2017)]

Cited by 10 publications

References 1 publication

Relationship between x-ray emission and absorption spectroscopy and the local H-bond environment in water

Relationship between x-ray emission and absorption spectroscopy and the local H-bond environment in water

Compressibility Anomalies in Stretched Water and Their Interplay with Density Anomalies

Glass polymorphism and liquid–liquid phase transition in aqueous solutions: experiments and computer simulations

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