Spatially inhomogeneous bimodal inherent structure of simulated liquid water.

In the supercooled regime at elevated pressure two forms of liquid water, high-density (HDL) and low-density (LDL), have been proposed to be separated by a coexistence line ending at a critical point, but a connection to water at ambient conditions has been lacking. Here we perform large-scale molecular dynamics simulations and demonstrate that the underlying potential energy surface gives a strictly bimodal characterization of the molecules at all temperatures and pressures, including the biologically and technologically important ambient regime, as spatially inhomogeneous either LDL- or HDL-like with a 3 : 1 predominance for HDL under ambient conditions. The Widom line in the supercooled regime, where maximal structural fluctuations take place, coincides with a 1 : 1 distribution. Although our results are based on molecular dynamics force-field simulations the close agreement with recent analyses of experimental X-ray spectroscopy and scattering data indicates a unified description also of real liquid water covering supercooled to ambient conditions.

• Publication year

  2011

• Venue

  Physical Chemistry, Chemical Physics - PCCP

• Publication date

  2011-06-24

• Fields of study

  Medicine, Physics, Chemistry

• Identifiers
  DOI 10.1039/c1cp22076darXiv 1106.5038PMID 21915406
• External record

  Open on Semantic Scholar

• Source metadata

  Semantic Scholar, PubMed

• No claims are published for this paper.

• No concepts are published for this paper.

• Enhanced small-angle scattering connected to the Widom line in simulations of supercooled water.

  2011cited by this paper
• Quantitative investigation of the two-state picture for water in the normal liquid and the supercooled regime

  2011cited by this paper
• Note: Equation of state and compressibility of supercooled water: simulations and experiment.

  2011cited by this paper
• Mixturelike behavior near a liquid-liquid phase transition in simulations of supercooled water.

  2011cited by this paper
• Perspective on the structure of liquid water

  2011cited by this paper
• Density hysteresis of heavy water confined in a nanoporous silica matrix

  2011cited by this paper
• Recent water myths

  2010cited by this paper
• The Widom line as the crossover between liquid-like and gas-like behaviour in supercritical fluids

  2010cited by this paper
• Widom line and the liquid-liquid critical point for the TIP4P/2005 water model.

  2010cited by this paper
• Is ambient water inhomogeneous on the nanometer-length scale?

  2010cited by this paper
• Reply to Soper et al.: Fluctuations in water around a bimodal distribution of local hydrogen-bonded structural motifs

  2010cited by this paper
• High resolution X-ray emission spectroscopy of water and its assignment based on two structural motifs

  2010cited by this paper
• Small-angle scattering and the structure of ambient liquid water

  2010cited by this paper
• The structure of ambient water

  2010cited by this paper
• Volume of supercooled water under pressure and the liquid-liquid critical point.

  2010cited by this paper
• Increasing correlation length in bulk supercooled H2O, D2O, and NaCl solution determined from small angle x-ray scattering.

  2010cited by this paper
• Theoretical Approximations to X-Ray Absorption Spectroscopy of Liquid Water and Ice

  2010cited by this paper
• X-ray absorption spectroscopy and X-ray Raman scattering of water and ice; an experimental view

  2010cited by this paper
• The glass transition and relaxation behavior of bulk water and a possible relation to confined water.

  2010cited by this paper
• Anomalies in water as obtained from computer simulations of the TIP4P/2005 model: density maxima, and density, isothermal compressibility and heat capacity minima

  2009cited by this paper
• Appearance of a Fractional Stokes-Einstein Relation in Water and a Structural Interpretation of Its Onset

  2009cited by this paper
• The inhomogeneous structure of water at ambient conditions

  2009cited by this paper
• Evidence of a two-state picture for supercooled water and its connections with glassy dynamics

  2009cited by this paper
• Insights into Phases of Liquid Water from Study of Its Unusual Glass-Forming Properties

  2008cited by this paper
• Effect of hydrogen bond cooperativity on the behavior of water

  2008cited by this paper
• High resolution X-ray emission spectroscopy of liquid water : The observation of two structural motifs

  2008cited by this paper
• GROMACS: Fast, flexible, and free

  2005cited by this paper
• A general purpose model for the condensed phases of water: TIP4P/2005.

  2005cited by this paper
• Relation between the Widom line and the dynamic crossover in systems with a liquid-liquid phase transition.

  2005cited by this paper
• The Structure of the First Coordination Shell in Liquid Water

  2004cited by this paper
• Supercooled and glassy water

  2003cited by this paper
• The interpretation of X-ray absorption spectra of water and ice

  2002cited by this paper
• Structures of high and low density amorphous ice by neutron diffraction.

  2002cited by this paper
• Supercooled liquids and the glass transition

  2001cited by this paper
• Simple physical model of liquid water

  2000cited by this paper
• Structures of high-density and low-density water

  2000cited by this paper
• Singularity-free interpretation of the thermodynamics of supercooled water.

  1998cited by this paper
• Molecular scale precursor of the liquid–liquid phase transition of water

  1998cited by this paper
• Decompression-induced melting of ice IV and the liquid–liquid transition in water

  1998cited by this paper
• The relationship between liquid, supercooled and glassy water

  1998cited by this paper
• Growth and collapse of structural patterns in the hydrogen bond network in liquid water

  1996cited by this paper
• X‐ray scattering in liquid water at pressures of up to 7.7 kbar: Test of a fluctuation model

  1994cited by this paper
• Particle mesh Ewald: An N⋅log(N) method for Ewald sums in large systems

  1993cited by this paper
• Phase behaviour of metastable water

  1992cited by this paper
• The structure

  1992cited by this paper
• Enhanced density fluctuations in water analyzed by neutron scattering.

  1989cited by this paper
• X-ray study of high-density amorphous water.

  1986cited by this paper
• Canonical dynamics: Equilibrium phase-space distributions.

  1985cited by this paper
• A molecular dynamics method for simulations in the canonical ensemble

  1984cited by this paper
• Packing Structures and Transitions in Liquids and Solids

  1984cited by this paper
• Stability-limit conjecture. An interpretation of the properties of water

  1982cited by this paper
• Heat capacity of water at extremes of supercooling and superheating. Technical report

  1981cited by this paper
• Polymorphic transitions in single crystals: A new molecular dynamics method

  1981cited by this paper
• Enhanced Density Fluctuations in Supercooled H 2 O, D 2 O, and Ethanol-Water Solutions: Evidence from Small-Angle X-Ray Scattering

  1981cited by this paper

• Tuning Water Density Fluctuations with Surface-Charged Colloidal Nanoparticles Probed by Luminescence.

  2025cites this paper
• Statistical Mechanical Theory of Liquid Water.

  2025cites this paper
• Structural Origin of Dynamic Heterogeneity in Supercooled Liquids

  2025cites this paper
• TIP 4 P 2005 Ice : Simulating water with two molecular states.

  2025cites this paper
• Atomic-Level Exploration of Local Structural Heterogeneity in Liquid Ga-In Alloys Using a Machine Learning Potential.

  2025cites this paper
• The water bimodal inherent structure and the liquid-liquid transition as proposed by the experimental density data.

  2024cites this paper
• Beyond Local Structures in Critical Supercooled Water through Unsupervised Learning.

  2024cites this paper
• Unraveling thermodynamic anomalies of water: A molecular simulation approach to probe the two-state theory with atomistic and coarse-grained water models.

  2024cites this paper
• Study of Protein Hydration Water with the V4S Structural Index: Focus on Binding Site Description.

  2024cites this paper
• Supercritical density fluctuations and structural heterogeneity in supercooled water-glycerol microdroplets

  2024influential citation
• IceCoder: Identification of Ice Phases in Molecular Simulation Using Variational Autoencoder.

  2024cites this paper
• Unraveling the dynamic slowdown in supercooled water: The role of dynamic disorder in jump motions.

  2024cites this paper
• A Unified Description of the Liquid Structure, Static and Dynamic Anomalies, and Criticality of TIP4P/2005 Water by a Hierarchical Two-State Model.

  2023cites this paper
• Water model for hydrophobic cavities: structure and energy from quantum-chemical calculations.

  2023cites this paper
• Quantum Electrodynamics Coherence and Hormesis: Foundations of Quantum Biology

  2023cites this paper
• A statistical mechanical model of supercooled water based on minimal clusters of correlated molecules.

  2023cites this paper
• Structural relaxation of water during rapid cooling from ambient temperatures.

  2023cites this paper
• Inherent structures of water using fully ab initio simulations.

  2023cites this paper
• The Dramatic Effect of Water Structure on Hydration Forces and the Electrical Double Layer

  2023cites this paper
• Dynamic Heterogeneity and Kovacs' Memory Effects in Supercooled Water.

  2023cites this paper
• Hydrogen bonded configurations in liquid water and their correlations with local tetrahedral structures

  2023cites this paper
• Temperature Dependence of Hydrogen Bond Networks of Liquid Water: Thermodynamic Properties and Structural Heterogeneity from Topological Descriptors.

  2023cites this paper
• Isotope effects on the structural transformation and relaxation of deeply supercooled water.

  2022cites this paper
• Is It Possible to Follow the Structural Evolution of Water in "No-Man's Land" Using a Pulsed-Heating Procedure?

  2022cites this paper
• Correlated Fluctuations of Structural Indicators Close to the Liquid–Liquid Transition in Supercooled Water

  2022cites this paper
• Protein hydration water: focus on low density and high density local structures upon cooling

  2022cites this paper
• A journey into the local structural order of liquid water: from the insights earned by geometrically-inspired descriptors to the development of a brand new energy-based indicator

  2022cites this paper
• Thermodynamics and structure of supercooled water. II.

  2022cites this paper
• Manifestations of the structural origin of supercooled water's anomalies in the heterogeneous relaxation on the potential energy landscape.

  2022cites this paper
• Correlated Local Fluctuations in the Hydrogen Bond Network of Liquid Water.

  2022cites this paper
• Simulation and theoretical analysis of the origin of the temperature of maximum density of water

  2022cites this paper
• Origin of the anomalous properties in supercooled water based on experimental probing inside “no-man's land”

  2022cites this paper
• Structural Changes of Interfacial Water upon Fluid-Ripple-Gel Phase Transitions of Bilayers

  2022cites this paper
• Structural characteristics of low-density environments in liquid water.

  2022cites this paper
• The local structure of water from combining diffraction and X-ray spectroscopy

  2022cites this paper
• Interpretation of the X-Ray Emission Spectra of Liquid Water through Temperature and Isotope Dependence.

  2022cites this paper
• A new one-site coarse-grained model for water: Bottom-up many-body projected water (BUMPer). II. Temperature transferability and structural properties at low temperature.

  2021cites this paper
• Topology and complexity of the hydrogen bond network in classical models of water

  2021cites this paper
• Advances in the study of supercooled water

  2021cites this paper
• High-Dimensional Fluctuations in Liquid Water: Combining Chemical Intuition with Unsupervised Learning.

  2021cites this paper
• Anomalous temperature dependence of the experimental x-ray structure factor of supercooled water.

  2021cites this paper
• Supercooled Water

  2021cites this paper
• Tetrahedral structure of supercooled water at ambient pressure and its influence on dynamic relaxation: Comparative study of water models

  2021cites this paper
• A hierarchical clustering method of hydrogen bond networks in liquid water undergoing shear flow

  2021cites this paper
• Dimensionality dependence of the Kauzmann temperature: A case study using bulk and confined water.

  2021cites this paper
• Structural relaxation and crystallization in supercooled water from 170 to 260 K

  2021cites this paper
• Structural aspects of an energy-based water classification index and the structure–dynamics link in glassy relaxation

  2021cites this paper
• On the existence of soliton-like collective modes in liquid water at the viscoelastic crossover

  2021cites this paper
• Relations between thermodynamics, structures, and dynamics for modified water models in their supercooled regimes.

  2021cites this paper
• X-Ray Studies of Water

  2020cites this paper
• Electrodynamic coherence as a biochemical and physical basis for emergence of perception , semantics , and adaptation in living systems

  2020cites this paper
• Electrodynamic Coherence as a Physical Basis for Emergence of Perception, Semantics, and Adaptation in Living Systems

  2020cites this paper
• Could Chemical Reaction at the Molecular Level Show Distinction between Two Liquid-Water States? Study of the Excited-State Water-Catalyzed Proton Transfer Reaction Provides a Clue.

  2020cites this paper
• Experimental tests for a liquid-liquid critical point in water

  2020cites this paper
• The anomalies and criticality of liquid water

  2020cites this paper
• Anisotropic X-Ray Scattering of Transiently Oriented Water.

  2020cites this paper
• Decoding a Percolation Phase Transition of Water at ~330 K with a Nanoparticle Ruler.

  2020cites this paper
• Instantaneous normal mode analysis for OKE reduced spectra of liquid and supercooled water: Contributions of low-density and high-density liquids

  2020cites this paper
• Structural features of high-local-density water molecules: Insights from structure indicators based on the translational order between the first two molecular shells.

  2019cites this paper
• Unravelling the contribution of local structures to the anomalies of water: The synergistic action of several factors.

  2019cites this paper
• Glass polymorphism in TIP4P/2005 water: A description based on the potential energy landscape formalism.

  2019cites this paper
• Revealing key structural features hidden in liquids and glasses

  2019cites this paper
• Translational and rotational dynamics of high and low density TIP4P/2005 water.

  2019cites this paper
• Intermediate range O-O correlations in supercooled water down to 235 K.

  2019cites this paper
• Is water one liquid or two?

  2019cites this paper
• The Boson peak interpretation and evolution in confined amorphous water

  2019cites this paper
• Liquid water structure from X-ray absorption and emission, NMR shielding and X-ray diffraction

  2019cites this paper
• Comparing the performance of two structural indicators for different water models while seeking for connections between structure and dynamics in the glassy regime.

  2019cites this paper
• Homogeneous nucleation of ferroelectric ice crystal driven by spontaneous dipolar ordering in supercooled TIP5P water.

  2019cites this paper
• A proposal for the structure of high- and low-density fluctuations in liquid water.

  2019cites this paper
• Radial distribution functions of water: Models vs experiments.

  2019cites this paper
• Temperature dependent anomalous fluctuations in water: shift of ≈1 kbar between experiment and classical force field simulations

  2019cites this paper
• Temperature dependence analysis of the NIR spectra of liquid water confirms the existence of two phases, one of which is in a coherent state

  2019cites this paper
• Proving coexistence of ice‐like and quartz‐like structure in localized liquid water by stimulated Raman scattering

  2019cites this paper
• Glass polymorphism and liquid-liquid phase transition in aqueous solutions: experiments and computer simulations.

  2019cites this paper
• Dielectric permittivity of aqueous solutions of electrolytes probed by THz time-domain and FTIR spectroscopy

  2019cites this paper
• Reversible structural transformations in supercooled water from 135 to 245 K

  2019cites this paper
• Direct evidence in the scattering function for the coexistence of two types of local structures in liquid water.

  2019cites this paper
• Reversible structural transformations in supercooled liquid water from 135 to 245 K

  2019cites this paper
• Revealing key structural features hidden in liquids and glasses

  2019cites this paper
• Impact of local symmetry breaking on the physical properties of tetrahedral liquids

  2018cites this paper
• Communication: Diffusion constant in supercooled water as the Widom line is crossed in no man's land.

  2018cites this paper
• Water Is a Cagey Liquid.

  2018cites this paper
• Potential energy landscape of TIP4P/2005 water.

  2018cites this paper
• Relationship between x-ray emission and absorption spectroscopy and the local H-bond environment in water.

  2018cites this paper
• Solvation Layer of Antifreeze Proteins Analyzed with a Markov State Model.

  2018cites this paper
• Microscopic structural descriptor of liquid water.

  2018cites this paper
• Water-like anomalies as a function of tetrahedrality

  2018cites this paper
• High density liquid structure enhancement in glass forming aqueous solution of LiCl.

  2018cites this paper
• Effects of the bond polarity on the structural and dynamical properties of silica-like liquids.

  2018cites this paper
• Viscosity and real-space molecular motion of water: Observation with inelastic x-ray scattering.

  2018cites this paper
• Structure and hydrogen bonding at the limits of liquid water stability

  2018cites this paper
• A Two-State Picture of Water and the Funnel of Life

  2018cites this paper
• Crucial role of fragmented and isolated defects in persistent relaxation of deeply supercooled water.

  2018cites this paper
• The multiple local structures in liquid water

  2017cites this paper
• Maxima in the thermodynamic response and correlation functions of deeply supercooled water

  2017cites this paper
• How Water’s Properties Are Encoded in Its Molecular Structure and Energies

  2017cites this paper
• Large-Scale Structure and Hyperuniformity of Amorphous Ices.

  2017cites this paper
• Temperature-dependent vibrational spectra and structure of liquid water from classical and quantum simulations with the MB-pol potential energy function.

  2017cites this paper
• Common behaviors associated with the glass transitions of water-like models.

  2017cites this paper