Ab initio molecular dynamics simulations of liquid water using high quality meta-GGA functionals

Pestana, Luis Ruiz; Mardirossian, Narbe; Head‐Gordon, Martin; Head‐Gordon, Teresa

doi:10.1039/c6sc04711d

Cited by 125 publications

(158 citation statements)

References 133 publications

(150 reference statements)

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“…by Lin et al [65], and has been related to improper description of the curvatures of potential energy surfaces. Recently, Pestana et al have demonstrated similar effects in BOMD simulations of liquid water by comparing the performance of dispersioncorrected GGA with high quality meta-GGA functionals [66]. More proper modeling of the vibrational response would, hence, call for the use of more advanced approximations to the exchange-correlation functional, possibly by employing non-local hybrid functionals.…”

Section: Inelastic Neutron Scatteringmentioning

confidence: 90%

Hydrogen dynamics in solid formic acid: insights from simulations with quantum colored-noise thermostats

Drużbicki

Krzystyniak

Hollas

et al. 2018

J. Phys.: Conf. Ser.

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Abstract. With an increase of computational capabilities, ab initio molecular dynamics becomes the natural choice for exploring the nuclear dynamics of solids. As based on classical mechanics, the validity of this approach is, in-principle, limited to the high-T regime, whilst low-temperature simulations require inclusion of quantum effects. The methods commonly used to account for nuclear quantum effects are based on the path-integral formalism, which become, however, particularly time consuming when high accuracy methods are used for calculating forces. Recently, new efficient alternative approaches to account for quantum nature of nuclei have been proposed, using so-called quantum thermostats. In this work, we examine the simulations performed with the quantum colored-noise thermostat introduced by Ceriotti [Phys. Rev. Lett., 103:030603, 2009]. We present the tests of portable implementation of the quantum thermostat in the ABIN program, which has been extended to periodic systems through the interface to CASTEP, a leading spectroscopy-oriented plane-wave density functional theory code. The range of applicability of quantum-thermostatted molecular dynamics simulations for the interpretation of neutron scattering data was examined and compared to classical molecular dynamics and lattice-dynamics simulations, using solid formic acid case as a test bed. We find that the approach is particularly useful for the modeling of low-temperature inelastic neutron scattering spectra as well as provides some theoretical estimate for the low-limit of the mean kinetic energy. While finding the quantum-thermostat to seriously affect the dynamic properties of the title system, we illustrate to which extent the unperturbed response can be successfully recovered. IntroductionMolecular dynamics (MD) has evolved into a powerful numerical method to investigate structural and dynamical properties of condensed matter [1]. For an atom, these calculations are, however, only valid in the classical limit, i.e. for temperatures safely above the Debye temperature that signals the onset of quantum effects. The Debye temperature is often of the order of few hundred Kelvins and nuclear quantum effects (NQEs) are thus indeed important over a wide range of temperatures [2,3].Quantum fluctuations stemming from the Heisenberg uncertainty principle make the energy of a particle at 0 K higher than a the potential energy minimum, leading to a concept of zero point energy (ZPE) (see Fig. 1). While ZPE reflects the quantum nature of atomic motion, it can be approximately accounted for by lattice-dynamics calculations, which, by definition, are based on the quantum harmonic oscillator model.

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Section: Inelastic Neutron Scatteringmentioning

confidence: 90%

Hydrogen dynamics in solid formic acid: insights from simulations with quantum colored-noise thermostats

Drużbicki

Krzystyniak

Hollas

et al. 2018

J. Phys.: Conf. Ser.

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“…65 This finding is consistent with a recent calculation of water clusters up to pentamer revealing that revPBE-D3 benefits from a subtle cancellation of error and that more accurate meta-GGA functionals in conjunction with NQE will provide the correct description of liquid water. 66 In order to ascertain differences between the empirical and the DFT-based interaction potentials for water, we have investigated the local structure of ambient water by looking into the distribution of the d 5 order parameter that represents the distance of the 5 th nearest neighbor from a tagged water molecule. We demonstrated that this order parameter probes the local heterogeneity of water and demonstrates that DFT based potentials exhibit a broad range of local environments, in contrast to the empirical models.…”

Section: Discussionmentioning

confidence: 99%

Mass density fluctuations in quantum and classical descriptions of liquid water

Galib

Duignan

Misteli

et al. 2017

The Journal of Chemical Physics

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First principles molecular dynamics simulation protocol is established using revised functional of Perdew-Burke-Ernzerhof (revPBE) in conjunction with Grimme's third generation of dispersion (D3) correction to describe properties of water at ambient conditions. This study also demonstrates the consistency of the structure of water across both isobaric (NpT) and isothermal (NVT) ensembles. Going beyond the standard structural benchmarks for liquid water, we compute properties that are connected to both local structure and mass density fluctuations that are related to concepts of solvation and hydrophobicity. We directly compare our revPBE results to the Becke-Lee-Yang-Parr (BLYP) plus Grimme dispersion corrections (D2) and both the empirical fixed charged model (SPC/E) and many body interaction potential model (MB-pol) to further our understanding of how the computed properties herein depend on the form of the interaction potential.

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“…Although recent AIMD simulations of liquid water with B97M-rV have already yielded encouraging results across a large set of water properties 29 , it remains to further test the B97M-rV density functional for solids, liquids, and interfaces in order to see if its demonstrated accuracy for various molecular interactions extends to properties that are significantly different from those used to train its parameters.…”

Section: Discussionmentioning

confidence: 99%

Use of the rVV10 Nonlocal Correlation Functional in the B97M-V Density Functional: Defining B97M-rV and Related Functionals

Mardirossian

Pestana

Womack

et al. 2016

J. Phys. Chem. Lett.

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100

136

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The VV10 and rVV10 nonlocal correlation functionals are consistently implemented and assessed, with the goal of determining if the rVV10 nonlocal correlation functional can replace the VV10 nonlocal correlation functional in the recently developed B97M-V density functional, to give the B97M-rV density functional. Along the way, four density functionals are simultaneously tested: VV10, rVV10, B97M-V, and B97M-rV. An initial assessment is carried out across the S22 data set, and the short-range damping variable, b, is varied for all four density functionals in order to determine the sensitivity of the functionals to the empirical parameter. The results of this test indicate that a value of b = 6 (fortuitously the same as that in B97M-V) is suitable for B97M-rV. The functionals are then compared across an extensive database of interaction energies, and it is demonstrated that B97M-rV either matches or outperforms B97M-V for all of the tests considered. Finally, the optimization of b across the S22 data set is extended to two range-separated hybrid density functionals, ωB97X-V and ωB97M-V, and a value of b = 6.2 is recommended for both ωB97X-rV and ωB97M-rV.

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Ab initio molecular dynamics simulations of liquid water using high quality meta-GGA functionals

Cited by 125 publications

References 133 publications

Hydrogen dynamics in solid formic acid: insights from simulations with quantum colored-noise thermostats

Hydrogen dynamics in solid formic acid: insights from simulations with quantum colored-noise thermostats

Mass density fluctuations in quantum and classical descriptions of liquid water

Use of the rVV10 Nonlocal Correlation Functional in the B97M-V Density Functional: Defining B97M-rV and Related Functionals

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