Hydrogen bonded configurations in liquid water and their correlations with local tetrahedral structures

Muthachikavil, Aswin V.; Peng, Baoliang; Kontogeorgis, Georgios M.

doi:10.1080/00268976.2023.2202265

Molecular Physics

2023

DOI: 10.1080/00268976.2023.2202265

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Hydrogen bonded configurations in liquid water and their correlations with local tetrahedral structures

Aswin V. Muthachikavil

Baoliang Peng

Georgios M. Kontogeorgis

Abstract: We compared the temperature trend of the fraction of hydrogen-bonded configurations estimated in our simulations using the iAMOEBA water model with the values reported by Gartner et al, using the MB-POL water model. The MB-POL water model is a many-body forcefield for simulation of water which captures the structure and properties of water very well, albeit being computationally expensive [1]. As can be seen from fig. S1, the temperature trends of different hydrogen-bonded configurations (when all hydrogen bon… Show more

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2024

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Cited by 2 publications

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Prediction of water anomalous properties by introducing the two-state theory in SAFT

Novak,

Liang,

Kontogeorgis

2024

The Journal of Chemical Physics

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Water is one of the most abundant substances on earth, but it is still not entirely understood. It shows unusual behavior, and its properties present characteristic extrema unlike any other fluid. This unusual behavior has been linked to the two-state theory of water, which proposes that water forms different clusters, one with a high density and one with a low density, which may even form two distinct phases at low temperatures. Models incorporating the two-state theory manage to capture the unusual extrema of water, unlike traditional equations of state, which fail. In this work, we have derived the framework to incorporate the two-state theory of water into the Statistical-Associating-Fluid-Theory (SAFT). More specifically, we have assumed that water is an ideal solution of high density water molecules and low density water molecules that are in chemical equilibrium. Using this assumption, we have generalized the association term SAFT to allow for the simultaneous existence of the two water types, which have the same physical parameters but different association properties. We have incorporated the newly derived association term in the context of the Perturbed Chain-SAFT (PC-SAFT). The new model is referred to as PC-SAFT-Two-State (PC-SAFT-TS). Using PC-SAFT-TS, we have succeeded in predicting the characteristic extrema of water, such as its density and speed of sound maximum, etc., without loss of accuracy compared to the original PC-SAFT. This new framework is readily extended to mixtures, and PC-SAFT-TS manages to capture the solubility minimum of hydrocarbons in water in a straightforward manner.

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Prediction of water anomalous properties by introducing the two-state theory in SAFT

Novak,

Liang,

Kontogeorgis

2024

The Journal of Chemical Physics

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Unraveling thermodynamic anomalies of water: A molecular simulation approach to probe the two-state theory with atomistic and coarse-grained water models

Muthachikavil,

Sun,

Peng

et al. 2024

The Journal of Chemical Physics

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Thermodynamic and dynamic anomalies of water play a crucial role in supporting life on our planet. The two-state theory attributes these anomalies to a dynamic equilibrium between locally favored tetrahedral structures (LFTSs) and disordered normal liquid structures. This theory provides a straightforward, phenomenological explanation for water’s unique thermodynamic and dynamic characteristics. To validate this two-state feature, it is critical to unequivocally identify these structural motifs in a dynamically fluctuating disordered liquid. In this study, we employ a recently introduced structural parameter (θavg) that characterizes the local angular order within the first coordination shell to identify these LFTSs through molecular dynamics simulations. We employ both realistic water models with a liquid–liquid critical point (LLCP) and a coarse-grained water model without an LLCP to study water’s anomalies in low-pressure regions below 2 kbar. The two-state theory consistently describes water’s thermodynamic anomalies in these models, both with and without an LLCP. This suggests that the anomalies predominantly result from the two-state features rather than criticality, particularly within experimentally accessible temperature–pressure regions.

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Hydrogen bonded configurations in liquid water and their correlations with local tetrahedral structures

Cited by 2 publications

References 77 publications

Prediction of water anomalous properties by introducing the two-state theory in SAFT

Prediction of water anomalous properties by introducing the two-state theory in SAFT

Unraveling thermodynamic anomalies of water: A molecular simulation approach to probe the two-state theory with atomistic and coarse-grained water models

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