相关论文: Electronic structure of water from Koopmans-compli…
During compression of a water dimer calculated with high-precision first-principles methods, the trends of H-bond and O-H bond lengths show quantum effect of the electronic structure. We found that the H-bond length keeps decreasing, while…
In the last decade, computational studies of liquid water have mostly concentrated on ground state properties. However recent spectroscopic measurements have been used to infer the structure of water, and the interpretation of optical and…
The structure of liquid water at ambient conditions is studied in ab initio molecular dynamics simulations using van der Waals (vdW) density-functional theory, i.e. using the new exchange-correlation functionals optPBE-vdW and vdW-DF2.…
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…
An accurate ab initio theory of the H-bond structure of liquid water requires a high-level exchange correlation approximation from density functional theory. Based on the liquid structures modeled by ab initio molecular dynamics by using…
Oxygen K-edge X-ray absorption spectra of liquid water are computed based on the configurations from advanced ab initio molecular dynamics simulations, as well as an electron excitation theory from the GW method. One one hand, the molecular…
The local structure of liquid water as a function of temperature is a source of intense research. This structure is intimately linked to the dynamics of water molecules, which can be measured using Raman and infrared spectroscopies. The…
We analyze and compare the structural, dynamical, and electronic properties of liquid water next to prototypical metals including Pt, graphite, and graphene. Our results are built on Born-Oppenheimer molecular dynamics (BOMD) generated…
Hydrophobic solutes significantly alters water hydrogen bond network. The local alteration of solvation struc-tures get reflected in the vibrational spectroscopic signal. Although it is possible to detect this microscopicfeatures by modern…
Hydrogen bond (H-bond) covalency has recently been observed in ice and liquid water, while the penetrating molecular orbitals (MOs) in the H-bond region of most typical water dimer system, (H2O)2, have also been discovered. However,…
We report an analysis of the stretching peak appearing in the IR experimental spectra of liquid water. In the literature, ATR-IR spectroscopic measurements were repeatedly performed in a wide range of temperature and gave rise to a lively…
The network connectivity in liquid water is revised in terms of electronic signatures of hydrogen bonds (HBs) instead of geometric criteria, in view of recent X-ray absorption studies. The analysis is based on ab initio molecular-dynamics…
Over the past decade we have developed Koopmans functionals, a computationally efficient approach for predicting spectral properties with an orbital-density-dependent functional framework. These functionals impose a generalized piecewise…
There is a long-standing question about the molecular configuration of interfacial water molecules in the proximity of solid surfaces, particularly carbon atoms which play a crucial role in electrochemistry and biology. In this study, the…
Koopmans-compliant functionals provide an orbital-density-dependent framework for an accurate evaluation of spectral properties; they are obtained by imposing a generalized piecewise-linearity condition on the total energy of the system…
Water is the liquid of life, thanks to its three-dimensional adaptive hydrogen (H)-bond network. Confinement of this network may lead to dramatic structural changes that influence chemical and physical transformations. Although confinement…
We evaluate the density of states of the quenched normal modes of ST2 water, and their statistical fluctuations, for a range of densities spanning three regimes of behavior of a hydrogen bonded liquid: a lower-density regime of random…
X-ray absorption spectroscopy (XAS) is a powerful experimental technique to probe the local order in materials with core electron excitations. Experimental interpretation requires supporting theoretical calculations. For water, these…
Numerous studies have identified large quantum mechanical effects in the dynamics of liquid water. In this paper, we suggest that these effects may have been overestimated due to the use of rigid water models and flexible models in which…
The optical spectrum of liquid water is analyzed by subsystem time-dependent density functional theory. We provide simple explanations for several important (and so far elusive) features. Due to the disordered environment surrounding each…