A Quantum Theoretical Basis for Some Spectra – Structure Correlations in Crystalline Hydrates

Starting with the perturbation theory and the Hellmann-Feynmann theorem, an attempt was made to derive a fundamental theoretical basis for some frequency – structure correlations in crystalline hydrates. It was found that within a few reasonable approximations, a satisfactory theoretical background may be found for the νOH(OD) versus RO⋅⋅⋅O, as well as for the –2XOH(OD) versus νOH(OD) correlations (νOH(OD) is the spectroscopically measured wavenumber of the OH(OD) stretching vibration, RO⋅⋅⋅O is the hydrogen bond distance, and X is the anharmonicity of vibration). The OH(OD) oscillators were treated as mixed cubic – quartic anharmonic systems. The influence of hydrogen bonding on these oscillators was introduced through the changes in the harmonic diagonal force constants (as proposed by Sceats and Rice1), the other diagonal terms in the potential energy expression being regarded as practically unchanged in the course of the hydrogen bonding. The parameters obtained by empirical correlations, within the proposed model, describe the dependence of the intramolecular potential of the uncoupled OH(OD) species on the hydrogen bond strength

A Quantum Theoretical Basis for Some Spectra – Structure Correlations in Crystalline Hydrates

Starting with the perturbation theory and the Hellmann-Feynmann theorem, an attempt was made to derive a fundamental theoretical basis for some frequency – structure correlations in crystalline hydrates. It was found that within a few reasonable approximations, a satisfactory theoretical background may be found for the νOH(OD) versus RO⋅⋅⋅O, as well as for the –2XOH(OD) versus νOH(OD) correlations (νOH(OD) is the spectroscopically measured wavenumber of the OH(OD) stretching vibration, RO⋅⋅⋅O is the hydrogen bond distance, and X is the anharmonicity of vibration). The OH(OD) oscillators were treated as mixed cubic – quartic anharmonic systems. The influence of hydrogen bonding on these oscillators was introduced through the changes in the harmonic diagonal force constants (as proposed by Sceats and Rice1), the other diagonal terms in the potential energy expression being regarded as practically unchanged in the course of the hydrogen bonding. The parameters obtained by empirical correlations, within the proposed model, describe the dependence of the intramolecular potential of the uncoupled OH(OD) species on the hydrogen bond strength

A study of defect structures in Fe-alloyed ZnO: Morphology, magnetism, and hyperfine interactions

In order to study the effect of Fe cation substitution on the local structure, defect formation, and hyperfine interactions in ZnO, Mössbauer spectroscopy measurements of the microwave processed Zn1−xFexO (x=0.05, 0.10, 0.15, and 0.20) nanoparticles, together with ab initio calculations, were performed. Complementary information on the distribution of particle size and morphology, as well as magnetic properties, were obtained by X-ray diffraction, transmission electron microscopy, and squid-magnetometry. The selected model for analyzing the Mössbauer spectra of our samples is a distribution of quadrupole splittings. The fitting model with two Lorentz doublets was rejected due to its failure to include larger doublets. The Fe3+ ions do not yield magnetic ordering in the samples at room temperature. The results from first-principles calculations confirm that the major component of the Mössbauer spectra corresponds to the Fe-alloyed ZnO with Zn vacancy in the next nearest neighbor environment. The magnetic measurements are consistent with the description of the distribution of iron ions over the randomly formed clusters in the ZnO host lattice. While at room temperature all the samples are paramagnetic, magnetic interactions cause a transition into a cluster spin-glass state at low temperatures

Determining the dust environment of an unknown comet for a spacecraft flyby: The case of ESA’s Comet Interceptor mission

Context. An assessment of the dust environment of a comet is needed for data analysis and planning spacecraft missions, such as ESA’s Comet Interceptor (CI) mission. The distinctive feature of CI is that the target object will be defined shortly before (or even after) launch; as a result, the properties of the nucleus and dust environment are poorly constrained, and therefore make the assessment of the dust environment challenging. Aims. The main goal of the work is to provide realistic estimations of a dust environment based on very general parameters of possible target objects. Methods. Contemporary numerical models of a dusty-gas coma were used to obtain spatial distribution of dust for a given set of parameters. By varying parameters within a range of possible values, we obtained an ensemble of possible dust distributions. Then, this ensemble was statistically evaluated in order to define the most probable cases and hence reduce the dispersion. This ensemble can not only be used to estimate the likely dust abundance along a flyby trajectory of a spacecraft, for example, but also to quantify the associated uncertainty. Results. We present a methodology of the dust environment assessment for the case when the target comet is not known beforehand (or when its parameters are known with large uncertainty). We provide an assessment of dust environment for the CI mission. We find that the lack of knowledge of any particular comet results in very large uncertainties (~3 orders of magnitude) for the dust densities within the coma. The most sensitive parameters affecting the dust densities are the dust size distribution, the dust production rate, and coma brightness, often quantified by Afρ. Further, the conversion of a coma’s brightness (Afρ) to a dust production rate is poorly constrained. The dust production rate can only be estimated down to an uncertainty of ~0.5 orders of magnitude if the dust size distribution is known in addition to the Afρ. Conclusions. To accurately predict the dust environment of a poorly known comet, a statistical approach needs to be taken to properly reflect the uncertainties. This can be done by calculating an ensemble of comae covering all possible combinations within parameter space as shown in this work

Point defect-enhanced optical and photoelectrochemical water splitting activity of nanostructured Zn1-xFeyO(1-x+1.5y)

Even has been under study since 1935, zinc oxide (ZnO) based materials still attract a huge scientific attention. Owing to a wide band gap energy (3.37 eV at room temperature) and a large exciton binding energy (60 meV) ZnO has a variety of application, e.g. in electronics, optoelectronics, spintronics and photocatalysis. Besides, it has been shown that zinc oxide-based materials have a great potential as photoelectrocatalysts in the processes of water splitting, yielding an increased both photocurrent density and photoconversion efficiency. However, with a band gap energy of 3.37 eV, ZnO is restricted to absorb UV light only. This restriction can be overcome by modifying optical properties of zinc oxide particles. During the years different approaches have been applied to modify the visible light photocatalytic activity of ZnO materials, for example: (1) metal and nonmetal ion doping, (2) hydrogenation, (3) the incorporation of crystalline defects in the form of vacancies and interstitials, (4) the modification of particles morphology and surface topology, etc. In this study we employed 3d metal ion substitution to improve visible light-driven photoactivity of zinc oxide particles. We investigated the influence of Fe concentration in Zn1-xFeyO(1-x+1.5y) nanoparticles on crystal structure, textural, optical and photoelectrocatalytic properties. Zn1-xFeyO(1-x+1.5y) nanoparticles with nominally 5, 10, 15 and 20 at.% of Fe ions were synthesized by microwave processing of a precipitate. The crystal structure and phase purity of the samples were investigated by X-ray diffraction, Raman and ATR-FTIR spectroscopy. Mössbauer spectroscopy was carried out to clarify the valence state of the iron ions in the ZnO crystal structure. Effects of the iron ions concentration on particles morphology and texture properties were observed with field emission scanning electron microscopy (FE–SEM), transmission electron microscopy (TEM) with elemental mapping, and nitrogen adsorption–desorption isotherm, respectively. The optical properties were studied using UV–Vis diffuse reflectance and photoluminescence (PL) spectroscopy. Photoelectrochemical activity of the Zn1-xFeyO(1-x+1.5y) samples as anode material was evaluated by linear sweep voltammetry in Na2SO4 electrolyte; the oxygen evolution kinetics were determined and compared. In addition, a series of first principles calculations were performed to address the influence of the iron concentration on the electronic structure of Zn1-xFeyO(1-x+1.5y) samples

GIADA microbalance measurements on board Rosetta: submicrometer- to micrometer-sized dust particle flux in the coma of comet 67P/Churyumov-Gerasimenko

Context. From August 2014 to September 2016, Rosetta escorted comet 67P/Churyumov-Gerasimenko (67P) during its journey around the Sun. One of the aims of Rosetta was to characterize cometary activity and the consequent formation of dust flux structures in cometary comae. Aims: We characterize and quantify the submicrometer- to micrometer-sized dust flux that may be shaped in privileged directions within the coma of 67P inbound to and outbound from perihelion. Methods: The in situ dust-measuring instrument GIADA, part of the Rosetta/ESA payload, consisted of three subsystems, one of which was the Micro Balance Subsystem (MBS), composed of five quartz crystal microbalances. From May 2014 to September 2016, MBS measured the submicrometer- to micrometer-sized deposited dust mass every 5 min. Results: We characterized the submicrometer- to micrometer-sized dust mass flux in the coma of 67P. The anti-sunward and the radial direction are preferred, and the flux is higher in the anti-sunward direction. The measured cumulative dust mass in the anti-sunward direction is 2.38 ± 0.04 × 10-7 kg, and in the radial direction, it is 1.18 ± 0.02 × 10-7 kg. We explain the anti-sunward dust flux as the effect of nonuniform gas emission between the night- and dayside of the nucleus, which acts in combination with the solar radiation pressure. We compared the cumulated dust mass of particles ≤5 μm with particles ≥100 μm. The retrieved ratio of ≈2% implies a differential size distribution index of ≈-3.0, which confirms that particles of size ≥0.1 mm dominate the dust coma cross-section of 67P during the entire orbit. Conclusions: Submicrometer- to micrometer-sized dust mass flux measurements were made for the first time from the arising of cometary activity until its extinction. They indicate that these particles do not provide a substantial optical scattering in the coma of 67P with respect to the scattering caused by millimeter-sized particles. In addition, MBS data reveal that the measured dust flux is highly anisotropic: anti-sunward plus radial

D7.3 - Data Management Plan

This document describes the initial version of the Data Management Plan (DMP) for the WaPoDe project. The overall objective of the WaPoDe project is to synthetize materials with enhanced sensitivity, selectivity, and response time as electrochemical sensors (ECS) for detection and monitoring of different pharmaceutical and pesticide pollutants in water and to reduce ECS manufacturing costs. The focus of the WaPoDe project is on ZnO-based electrochemical sensors. The database will be developed under the WaPoDe project with the main purpose to summarize the WaPoDe research results on the types, properties, and application of ZnO-based nanoparticles as selective ECS. This initial DMP provides information on the data management principles that will be implemented during and for a certain period after the WaPoDe project completion. It is based on the Data Management Plan template (https://enspire.science/wp-content/uploads/2021/09/Horizon-Europe-Data-Management-Plan-Template.pdf) which follows the guidelines from Europe Horizon calls. This DMP will be regularly updated as the implementation of the project progresses. The draft DMP was developed within the project workpackages