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Path-integral ab initio molecular dynamics (PI-AIMD) calculations have been employed to probe the nature of chloride ion solvation in aqueous solution. Nuclear quantum effects (NQEs) are shown to weaken hydrogen bonding between the chloride…

化学物理 · 物理学 2021-01-13 Jianhang Xu , Zhaoru Sun , Chunyi Zhang , Mark DelloStritto , Michael L. Klein , Deyu Lu , Xifan Wu

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…

化学物理 · 物理学 2026-05-20 Michael Beerbaum , Julian Heske , Jure Gujt , 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…

化学物理 · 物理学 2020-11-03 Imre Bakó , Ádám Madarász , László Pusztai

Water molecules adsorbed on inorganic substrates play an important role in several technological applications. In the presence of light atoms in adsorbates, nuclear quantum effects (NQE) influence properties of these systems. In this work,…

化学物理 · 物理学 2017-12-06 Yair Litman , Davide Donadio , Michele Ceriotti , Mariana Rossi

We employ classical and ring polymer molecular dynamics simulations to study the effect of nuclear quantum fluctuations on the structure and the water exchange dynamics of aqueous solutions of lithium and fluoride ions. While we obtain…

化学物理 · 物理学 2015-06-23 David M. Wilkins , David E. Manolopoulos , Liem X. Dang

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…

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…

化学物理 · 物理学 2015-06-19 Lu Wang , Michele Ceriotti , Thomas E. Markland

Nuclear quantum effects (NQEs) on the structures and transport properties of dense liquid hydrogen at densities of 10-100 g/cm3 and temperatures of 0.1-1 eV are fully assessed using \textit{ab initio} path-integral molecular dynamics…

材料科学 · 物理学 2019-12-10 Dongdong Kang , Huayang Sun , Jiayu Dai , Zengxiu Zhao , Yong Hou , Jiaolong Zeng , Jianmin Yuan

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…

化学物理 · 物理学 2017-02-28 Ondrej Marsalek , Thomas E. Markland

At room temperature, the quantum contribution to the kinetic energy of a water molecule exceeds the classical contribution by an order of magnitude. The quantum kinetic energy (QKE) of a water molecule is modulated by its local chemical…

化学物理 · 物理学 2020-01-22 Lu Wang , Michele Ceriotti , Thomas E. Markland

In this study we investigate the nuclear quantum effects (NQEs) on the acidity constant (pKA) of liquid water isotopologues at the ambient condition by path integral molecular dynamics (PIMD) simulations. We compared simulations using a…

化学物理 · 物理学 2021-03-17 Bo Thomsen , Motoyuki Shiga

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…

材料科学 · 物理学 2013-03-28 M. A. Morales , J. M. McMahon , C. Pierleoni , D. M. Ceperley

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…

化学物理 · 物理学 2024-12-03 Nore Stolte , János Daru , Harald Forbert , Jörg Behler , Dominik Marx

We investigate the effect of nuclear quantum effects (NQEs) of hydrogen atoms on the elasticity of ice VII at high pressure and ambient temperature conditions using ab initio path-integral molecular dynamics (PIMD) calculations. We find…

材料科学 · 物理学 2024-07-09 Jun Tsuchiya , Motoyuki Shiga , Shinji Tsuneyuki , Elizabeth C. Thompson

Despite the inherently quantum mechanical nature of hydrogen bonding, it is unclear how nuclear quantum effects (NQEs) alter the strengths of hydrogen bonds. With this in mind, we use ab initio path integral molecular dynamics to determine…

化学物理 · 物理学 2016-11-22 Wei Fang , Ji Chen , Mariana Rossi , Yexin Feng , Xin-Zheng Li , Angelos Michaelides

We present Q-AMOEBA (CF), an enhanced version of the Q-AMOEBA polarizable model that integrates a geometry-dependent charge flux (CF) term while designed for an explicit treatment of nuclear quantum effects (NQE). The inclusion of CF…

化学物理 · 物理学 2025-06-05 Nastasia Mauger , Thomas Plé , Louis Lagardère , Simon Huppert , Jean-Philip Piquemal

Anion hydration is complicated by H-bond donation between neighboring water molecules in addition to H-bond donation to the anion. This situation can lead to competing structures for chemically simple clusters like (H$_2$O)$_n$Cl$^-$ and to…

化学物理 · 物理学 2021-10-04 A. Muralidharan , L. R. Pratt , M. I. Chaudhari , S. B. Rempe

Atomistic simulations based on the first-principles of quantum mechanics are reaching unprecedented length scales. This progress is due to the growth in computational power allied with the development of new methodologies that allow the…

材料科学 · 物理学 2021-05-19 Mariana Rossi

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…

化学物理 · 物理学 2015-04-21 Thomas Spura , Christopher John , Scott Habershon , Thomas D. Kühne

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…

化学物理 · 物理学 2014-02-13 Jeffrey M. McMahon , Miguel A. Morales , Brian Kolb , Timo Thonhauser
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