相关论文: Disentangling Structural Information From Core-lev…
We explore the sensitivity of several core-level spectroscopic methods to the underlying atomistic structure by using the water molecule as our test system. We first define a metric that measures the magnitude of spectral change as a…
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…
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…
The x-ray absorption spectra of water and ice are calculated with a many-body approach for electron-hole excitations. The experimental features, including the small effects of temperature change in the liquid, are quantitatively reproduced…
X-ray Raman spectra of liquid, sub- and super- critical water at the oxygen K-edge were measured, at densities 1.02 - 0.16 gcm^-3. Measurements were made along both an isotherm and an isochore passing near the critical point. As density is…
Machine learning can reveal new insights into X-ray spectroscopy of liquids when the local atomistic environment is presented to the model in a suitable way. Many unique structural descriptor families have been developed for this purpose.…
The isotope effects in x-ray absorption spectra of liquid water are studied by a many-body approach within electron-hole excitation theory. The molecular structures of both light and heavy water are modeled by path-integral molecular…
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…
While many vibrational Raman spectroscopy studies of liquid water have investigated the temperature dependence of the high-frequency O-H stretching region, few have analyzed the changes in the Raman spectrum as a function of temperature…
Absorption spectra of liquid water at 300 K are calculated from both classical and density functional theory molecular dynamics simulation data, which together span from 1 MHz to hundreds of THz, agreeing well with experimental data…
Liquids generally become more ordered upon cooling. However, it has been a long-standing debate on whether such structural ordering in liquid water takes place continuously or discontinuosly: continuum vs. mixture models. Here, by computer…
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…
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…
Two-dimensional spectroscopic techniques combining terahertz (THz), infrared (IR), and visible pulses offer a wealth of information about coupling among vibrational modes in molecular liquids, thus providing a promising probe of their local…
Theoretical optical and x-ray spectra of model structures of water and ice are calculated using a many-body perturbation theory, Bethe-Salpeter equation (BSE) approach implemented in the valence- and core-excitation codes AI2NBSE and OCEAN.…
We apply a recently developed technique utilizing machine learning for statistical analysis of computational nitrogen K-edge spectra of aqueous triglycine. This method, the emulator-based component analysis, identifies spectrally relevant…
Electronic transitions involving core-level orbitals offer a localized, atomic-site and element specific peek window into statistical systems such as molecular liquids. Although formally understood, the complex relation between structure…
The supra-molecular structure of a liquid is strongly connected to its dynamics which in turn controls macroscopic properties such as viscosity. Consequently, detailed knowledge about how this structure changes with temperature is essential…
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…
Transient X-ray absorption techniques can measure ultrafast dynamics of the elemental edges in a material or multiple layer junction, giving them immense potential for deconvoluting concurrent processes. However, the interpretation of the…