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Supercooled water is expected to exhibit a liquid--liquid phase transition between low- and high-density liquid states, possibly terminating in a liquid--liquid critical point in the experimentally difficult no man's land. Because the…

Chemical Physics · Physics 2026-05-20 Michael Beerbaum , Julian Heske , Jure Gujt , Thomas D. Kühne

Isotopic substitution, which can be realized both in experiment and computer simulations, is a direct approach to assess the role of nuclear quantum effects on the structure and dynamics of matter. Yet, the impact of nuclear quantum effects…

Chemical Physics · Physics 2024-12-03 Nore Stolte , János Daru , Harald Forbert , Jörg Behler , Dominik Marx

We have applied path integral simulations, in combination with new ab initio based water potentials, to investigate nuclear quantum effects in liquid water. Because direct ab initio path integral simulations are computationally expensive, a…

Chemical Physics · Physics 2015-04-21 Thomas Spura , Christopher John , Scott Habershon , Thomas D. Kühne

Corrections for nuclear quantum effects (NQE) have been calculated for classical molecular dynamics (MD) simulation models of light (H2O), heavy (D2O) and null (H1.28D0.72O) water. New path integral molecular dynamics (PIMD) simulations…

Chemical Physics · Physics 2020-11-03 Imre Bakó , Ádám Madarász , László Pusztai

The electronic properties and optical response of ice and water are intricately shaped by their molecular structure, including the quantum mechanical nature of hydrogen atoms. In spite of numerous studies appeared over decades, a…

We have applied path integral molecular dynamics simulations to investigate nuclear quantum effects on the vibrational dynamics of water molecules at the water-air interface. The instantaneous fluctuations in the frequencies of the O-H…

Chemical Physics · Physics 2022-02-22 Deepak Ojha , Andrés Henao , Frederik Zysk , Thomas D. Kühne

Understanding the reactivity and spectroscopy of aqueous solutions at the atomistic level is crucial for the elucidation and design of chemical processes. However, the simulation of these systems requires addressing the formidable…

Chemical Physics · Physics 2017-02-28 Ondrej Marsalek , Thomas E. Markland

Path-integral molecular dynamics simulations based on density functional theory employing exchange-correlation density functionals capable of treating nonlocal van der Waals (vdW) interactions self-consistently provide a remarkably accurate…

Chemical Physics · Physics 2014-02-13 Jeffrey M. McMahon , Miguel A. Morales , Brian Kolb , Timo Thonhauser

Hydrogen bonds are of paramount importance in the chemistry of clays, mediating the interaction between the clay surface and water, and for some materials between separate layers. It is well-established that the accuracy of a computational…

Chemical Physics · Physics 2022-03-14 Pawan J. K. Kurapothula , Sam Shepherd , David M. Wilkins

Nuclear quantum effects, such as zero-point energy and tunneling, cause significant changes to the structure and dynamics of hydrogen bonded systems such as liquid water. However, due to the current inability to simulate liquid water using…

Chemical Physics · Physics 2015-06-19 Lu Wang , Michele Ceriotti , Thomas E. Markland

Based on quantum-mechanical path-integral molecular dynamics simulations the impact of nuclear quantum effects on the vibrational and hydrogen bond dynamics in liquid water is investigated. The instantaneous fluctuations in the frequencies…

Soft Condensed Matter · Physics 2018-09-03 Deepak Ojha , Andres Henao , Thomas D Kühne

The inclusion of long-range electrostatics in atomistic machine learning (ML) is receiving increasing attention for achieving quantum-mechanical accuracy in predicting a wide range of molecular and material properties. However, there is…

Materials Science · Physics 2026-02-12 Federico Grasselli , Kevin Rossi , Stefano de Gironcoli , Andrea Grisafi

In this work, a path integral Car-Parrinello molecular dynamics simulation of liquid water is performed. It is found that the inclusion of nuclear quantum effects systematically improves the agreement of first principles simulations of…

Soft Condensed Matter · Physics 2009-11-13 Joseph A. Morrone , Roberto Car

Understanding nucleation from aqueous solutions is of fundamental importance in a multitude of fields, ranging from materials science to biophysics. The complex solvent-mediated interactions in aqueous solutions hamper the development of a…

Soft Condensed Matter · Physics 2023-08-28 Renjie Zhao , Ziyue Zou , John D. Weeks , Pratyush Tiwary

Using first-principles molecular dynamics, we study the influence of nuclear quantum effects (NQEs) and nonlocal exchange--correlation density functionals (DFs) near molecular dissociation in liquid hydrogen. NQEs strongly influence…

Materials Science · Physics 2013-03-28 M. A. Morales , J. M. McMahon , C. Pierleoni , D. M. Ceperley

Electron-hole excitation theory is used to unveil the role of nuclear quantum effects on the X-ray absorption spectral signatures of water, whose structure is computed via path-integral molecular dynamics with the MB-pol intermolecular…

Chemical Physics · Physics 2018-09-30 Zhaoru Sun , Lixin Zheng , Mohan Chen , Michael L. Klein , Francesco Paesani , Xifan Wu

Over the past decades, atomistic simulations of chemical, biological and materials systems have become increasingly precise and predictive thanks to the development of accurate and efficient techniques that describe the quantum mechanical…

Chemical Physics · Physics 2018-03-13 Thomas E. Markland , Michele Ceriotti

Hydrogen is the most abundant element in the universe. It is also the lightest and as such the most quantum of the elements, in the sense that quantum tunnelling, quantum delocalisation, and zero-point motion can be important. For practical…

Chemical Physics · Physics 2019-01-18 Wei Fang , Ji Chen , Yexin Feng , Xin-Zheng Li , Angelos Michaelides

To date X-ray spectroscopy has become a routine tool that can reveal highly local and element-specific information on the electronic structure of atoms in complex environments. Here, we focus on nuclear dynamical effects in X-ray spectra…

Chemical Physics · Physics 2016-08-12 Sven Karsten , Sergei D. Ivanov , Saadullah G. Aziz , Sergey I. Bokarev , Oliver Kühn

The most successful and popular machine learning models of atomic-scale properties derive their transferability from a locality ansatz. The properties of a large molecule or a bulk material are written as a sum over contributions that…

Chemical Physics · Physics 2020-01-08 Andrea Grisafi , Michele Ceriotti
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