Perspective: How good is DFT for water?

Abstract

Kohn-Sham density functional theory (DFT) has become established as an indispensable tool for investigating aqueous systems of all kinds, including those important in chemistry, surface science, biology and the earth sciences. Nevertheless, many widely used approximations for the exchange-correlation (XC) functional describe the properties of pure water systems with an accuracy that is not fully satisfactory. The explicit inclusion of dispersion interactions generally improves the description, but there remain large disagreements between the predictions of different dispersion-inclusive methods. We present here a review of DFT work on water clusters, ice structures and liquid water, with the aim of elucidating how the strengths and weaknesses of different XC approximations manifest themselves across this variety of water systems. Our review highlights the crucial role of dispersion in describing the delicate balance between compact and extended structures of many different water systems, including the liquid. By referring to a wide range of published work, we argue that the correct description of exchange-overlap interactions is also extremely important, so that the choice of semi-local or hybrid functional employed in dispersion-inclusive methods is crucial. The origins and consequences of beyond-2-body errors of approximate XC functionals are noted, and we also discuss the substantial differences between different representations of dispersion. We propose a simple numerical scoring system that rates the performance of different XC functionals in describing water systems, and we suggest possible future developments.

References in corpus (47)

• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Van der Waals Density Functional for General Geometries
• Gaussian Approximation Potentials: the accuracy of quantum mechanics, without the electrons
• A Higher-Accuracy van der Waals Density Functional
• Efficient implementation of a van der Waals density functional: Application to double-wall carbon nanotubes
• Nonlocal van der Waals density functional: The simpler the better
• Perspective: Advances and challenges in treating van der Waals dispersion forces in density functional theory
• A molecular perspective of water at metal interfaces
• Van der Waals Density Functional for Layered Structures
• Competing quantum effects in the dynamics of a flexible water model
• How van der Waals interactions determine the unique properties of water
• Nuclear quantum effects in water
• An Efficient and Accurate Car-Parrinello-like Approach to Born-Oppenheimer Molecular Dynamics
• What ice can teach us about water interactions: a critical comparison of the performance of different water models
• Continuum variational and diffusion quantum Monte Carlo calculations
• Towards an assessment of the accuracy of density functional theory for first principles simulations of water II
• The Individual and Collective Effects of Exact Exchange and Dispersion Interactions on the Ab Initio Structure of Liquid Water
• Density, structure and dynamics of water: the effect of Van der Waals interactions
• Ice XV: a new thermodynamically stable phase of ice
• i-PI: A Python interface for ab initio path integral molecular dynamics simulations
• On the accuracy of DFT exchange-correlation functionals for H bonds in small water clusters II: The water hexamer and van der Waals interactions
• Hydrogen bonds and van der Waals forces in ice at ambient and high pressures
• On how good DFT exchange-correlation functionals are for H bonds in small water clusters: Benchmarks approaching the complete basis set limit
• Electronic signature of the instantaneous asymmetry in the first coordination shell of liquid water
• To wet or not to wet? Dispersion forces tip the balance for water-ice on metals
• Network equilibration and first-principles liquid water
• Free energy of liquid water on the basis of quasi-chemical theory and ab initio molecular dynamics
• Anomalous Nuclear Quantum Effects in Ice
• On the Accuracy of van der Waals Inclusive Density-Functional Theory Exchange-Correlation Functionals for Ice at Ambient and High Pressures
• Local Structure Analysis in $Ab$ $Initio$ Liquid Water
• Isobaric first-principles molecular dynamics of liquid water with nonlocal van der Waals interactions
• Quantum fluctuations and isotope effects in ab initio descriptions of water
• A first principles simulation of rigid water
• Recent achievements in ab initio modelling of liquid water
• Energy benchmarks for water clusters and ice structures from an embedded many-body expansion
• Coupled cluster benchmarks of water monomers and dimers extracted from DFT liquid water: the importance of monomer deformations
• Ab-initio molecular dynamics simulation of liquid water by Quantum Monte Carlo
• Dissociation energy of the water dimer from Quantum Monte Carlo calculations
• Assessing the accuracy of quantum Monte Carlo and density functional theory for energetics of small water clusters
• Room temperature compressibility and diffusivity of liquid water from first principles
• Anharmonic nuclear motion and the relative stability of hexagonal and cubic ice
• vdW-DF Study of energetic, structural, and vibrational properties of small water clusters and ice Ih
• A Transferable H2O Interaction Potential Based on a Single Center Multipole Expansion: SCME
• The complex kinetics of the ice VI to ice XV hydrogen ordering phase transition
• On "the complete basis set limit" and plane-wave methods in first-principles simulations of water
• Electronic and Nuclear Quantum Effects on the Ice XI/Ice Ih Phase Transition

Cited by in corpus (88)

• Ab initio theory and modeling of water
• Unravelling CO adsorption on model single-atom catalysts
• Why does hydronium diffuse faster than hydroxide in liquid water?
• On the accuracy of the MB-pol many-body potential for water: Interaction energies, vibrational frequencies, and classical thermodynamic and dynamical properties from clusters to liquid water and ice
• Simulation and understanding of quantum crystals
• Dissolving salt is not equivalent to applying a pressure on water
• Pressure and stress tensor of complex anharmonic crystals within the stochastic self-consistent harmonic approximation
• Water Agglomerates on Fe3O4(001)
• Learning neural network potentials from experimental data via Differentiable Trajectory Reweighting
• Phase equilibrium of water with hexagonal and cubic ice using the SCAN functional
• Structural, Electronic, and Dynamical Properties of Liquid Water by ab initio Molecular Dynamics based on SCAN Functional within the Canonical Ensemble
• Mass Density Fluctuations in Quantum and Classical descriptions of Liquid Water
• Measuring surface charge: why experimental characterization and molecular modeling should be coupled
• Quantum-mechanical exploration of the phase diagram of water
• Interaction between water and carbon nanostructures: How good are current density functional approximations?
• Exploring the Absorption Spectrum of Simulated Water from MHz to the Infrared
• Viscosity in water from first-principles and deep-neural-network simulations
• Towards the ground state of molecules via diffusion Monte Carlo on neural networks
• The Excess Proton at the Air-Water Interface: The Role of Instantaneous Liquid Interfaces
• Evidence for Stable Square Ice from Quantum Monte Carlo
• How ice grows from premelting films and water droplets
• Vapor-liquid equilibrium of water with the MB-pol many-body potential
• Ab-initio Structure and Thermodynamics of the RPBE-D3 Water/Vapor Interface by Neural-Network Molecular Dynamics
• Insights into lithium manganese oxide-water interfaces using machine learning potentials
• How strongly do hydrogen and water molecules stick to carbon nanomaterials?
• The S66 noncovalent interactions benchmark reconsidered using explicitly correlated methods near the basis set limit
• Nanoconfinement Facilitates Reactions of Carbon Dioxide in Supercritical Water
• Decisive role of nuclear quantum effects on surface mediated water dissociation at finite temperature
• The physics of Empty Liquids: from Patchy particles to Water
• Double-layer ice from first principles
• Osmotic transport at the aqueous graphene and hBN interfaces: scaling laws from a unified, first principles description
• Predicting Properties of Periodic Systems from Cluster Data: A Case Study of Liquid Water
• Critical role of quantum dynamical effects in the Raman spectroscopy of liquid water
• Detailed crystallographic analysis of the ice VI to ice XV hydrogen ordering phase transition
• Fully First-Principles Surface Spectroscopy with Machine Learning
• Hydration of NH${}_4^{+}$ in Water: Bifurcated Hydrogen Bonding Structures and Fast Rotational Dynamics
• Learning from the Density to Correct Total Energy and Forces in First Principle Simulations
• DMC-ICE13: ambient and high pressure polymorphs of ice from Diffusion Monte Carlo and Density Functional Theory
• Entropy governs the structure and reactivity of water dissociation under electric fields
• Liquid Water through Density-Functional Molecular Dynamics: Plane-Wave vs Atomic-Orbital Basis Sets
• Predictive simulations of ionization energies of solvated halide ions with relativistic embedded Equation of Motion Coupled-Cluster Theory
• The Hopping Mechanism of the Hydrated Excess Proton and Its Contribution to Proton Diffusion in Water
• Common Cations are not Polarizable: Effects of Dispersion Correction on Hydration Structures from Ab Initio Molecular Dynamics
• Disentangling Structural Information From Core-level Excitation Spectra
• On the influence of water on THz vibrational spectral features of molecular crystals
• Self-Interaction Correction in Water-Ion Clusters
• Designing an All-Carbon Membrane for Water Desalination
• Diffusion-Oscillatory Dynamics in Liquid Water on Data of Dielectric Spectroscopy
• Small polarons and the Janus nature of ${\text{TiO}}_{\text{2}}(110)$
• Accurate diffusion coefficients of the excess proton and hydroxide in water via extensive ab initio simulations with different schemes
• Machine learning density functionals from the random-phase approximation
• Improved Ab Initio Molecular Dynamics by Minimal Biasing with Experimental Data
• The nature of three-body interactions in DFT: exchange and polarization effects
• Developing machine-learned potentials to simultaneously capture the dynamics of excess protons and hydroxide ions in classical and path integral simulations
• Influence of Local Defects on the Dynamics of O-H Bond Breaking and Formation on a Magnetite Surface
• Properties of the tetravalent actinide series in aqueous phase from a microscopic simulation automated engine
• Quasi-Chemical Theory for Anion Hydration and Specific Ion Effects: Cl${}^{-}$(aq) \emph{vs.} F${}^{-}$(aq)
• Uncertainty Quantification in First-Principles Predictions of Harmonic Vibrational Frequencies of Molecules and Molecular Complexes
• Molecular Polarizability of Water from the Local Dielectric Response Theory
• From fifty years ago, the birth of modern liquid-state science
• Structural and Dynamic Properties of Solvated Hydroxide and Hydronium Ions in Water from Ab Initio Modeling
• Random Phase Approximation Applied to Many-Body Noncovalent Systems
• Proton dynamics in high-pressure ice-VII from density functional theory
• Random phase approximation with exchange for an accurate description of crystalline polymorphism
• Lifshitz interaction can promote ice growth at water-silica interfaces
• Random-Phase Approximation in Many-Body Noncovalent Systems: Methane in a Dodecahedral Water Cage
• Assessment of elastic models in supercooled water: A molecular dynamics study with the TIP4P/2005f force field
• Multitask methods for predicting molecular properties from heterogeneous data
• Comparison of water models for structure prediction
• Machine learning potentials for complex aqueous systems made simple
• Size and Quality of Quantum Mechanical Data Sets for Training Neural Network Force Fields for Liquid Water
• The Wetting of H${}_2$O by CO${}_2$
• Hydrogen Bonding and Nuclear Quantum Effects in Clays
• Unveiling the hidden reaction kinetic network of carbon dioxide in supercritical aqueous solutions
• Raman and IR spectra of water under graphene nanoconfinement at ambient and extreme pressure-temperature conditions: a first-principles study
• Aqueous Solution Chemistry In Silico and the Role of Data Driven Approaches
• Basic stability tests of machine learning potentials for molecular simulations in computational drug discovery
• A neural network potential with self-trained atomic fingerprints: a test with the mW water potential
• Atomistic Simulations of Oxide-Water Interfaces using Machine Learning Potentials
• ${}^{27}\text{Al }$ NMR chemical shift of $\text{Al}(\text{OH}{)}_4^{-}$ from first principles. Assessment of error cancellation in NMR chemical shift computations in chemically distinct reference and targeted systems
• When Quantum Fluctuations Meet Structural Instabilities: The Isotope- and Pressure-Induced Phase Transition in the Quantum Paraelectric NaOH
• Ferroelectricity induced by the absorption of water molecules on double helix SnIP
• Self-learning path integral hybrid Monte Carlo with mixed ab initio and machine learning potentials for modeling nuclear quantum effects in water
• Using a monomer potential energy surface to perform approximate path integral molecular dynamics simulation of ab-initio water with near-zero added cost
• Thermodynamical study of N${}_2$ clathrate hydrate from DFT calculations
• Does Cosmological Evolution Select for Technology?
• A Denser Hydrogen Inferred from First-Principles Simulations Challenges Jupiter's Interior Models
• Connection between water's dynamical and structural properties: insights from ab initio simulations