相关论文: Quantum dynamics and spectroscopy of ab initio liq…

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…

Vibrational spectroscopy is key for probing the interplay between the structure and dynamics of aqueous systems. In order to map different regions of experimental spectra to the microscopic structure of a system, it is important to combine…

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…

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…

We calculate the x-ray absorption spectra of liquid water at ambient conditions and of hexagonal ice close to melting, using a static GW approach that includes approximately local field effects. Quantum dynamics of the nuclei is taken into…

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…

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…

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…

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…

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…

Spectroscopy is an indispensable tool in understanding the structures and dynamics of molecular systems. However computational modelling of spectroscopy is challenging due to the exponential scaling of computational complexity with system…

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…

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…

Modeling electronic systems is an important application for quantum computers. In the context of materials science, an important open problem is the computational description of chemical reactions on surfaces. In this work, we outline a…

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…

Exposing a molecule to intense light pulses may bring this molecule to a nonstationary quantum state, thus launching correlated dynamics of electronic and nuclear subsystems. Although much had been achieved in the understanding of…

Molecular dynamics simulations are indispensable for exploring the behavior of atoms and molecules. Grounded in quantum mechanical principles, quantum molecular dynamics provides high predictive power but its computational cost is dominated…

Understanding the Raman spectroscopy at the atomistic level is important for the elucidation of dynamical processes in liquid water. Because the polarizability (or its time derivative) is often a highly nonlinear function of coordinates…

The notion that large electric fields at the air-water interface catalyze spontaneous chemical reactions has sparked significant debate, with far reaching implications for atmospheric chemistry and interfacial reactivity. Using vibrational…

Including quantum mechanical effects on the dynamics of nuclei in the condensed phase is challenging, because the complexity of exact methods grows exponentially with the number of quantum degrees of freedom. Efforts to circumvent these…