相关论文: Quantum fluctuations and isotope effects in ab ini…
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…
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…
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…
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…
When two phases of water are at equilibrium, the ratio of hydrogen isotopes in each is slightly altered due to their different phase affinities. This isotopic fractionation process can be utilized to analyze water's movement in the world's…
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…
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…
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…
A possible role of quantum effects, such as tunneling and zero-point energy, in the structural dynamics of supercooled liquids is studied by dielectric spectroscopy. Presented results demonstrate that the liquids, bulk 3-methylpentane 3MP…
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…
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…
Event-by-event hydrodynamics, with fluctuating initial conditions, has shown to nicely reproduce several features of experimentally observed quantities in high-energy nuclear collisions. Here we discuss how it may help to understand, in a…
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…
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…
Nuclear quantum effects play critical roles in a variety of molecular processes, especially in systems that contain hydrogen and other light nuclei, such as water. For water at ambient conditions, nuclear quantum effects are often…
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…
Quantum fluctuations or other moments of a state contribute to energy expectation values and can imply interesting physical effects. In quantum cosmology, they turn out to be important for a discussion of density bounds and instabilities of…
A comprehensive microscopic understanding of ambient liquid water is a major challenge for $ab$ $initio$ simulations as it simultaneously requires an accurate quantum mechanical description of the underlying potential energy surface (PES)…
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…
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…