Assessing temperature effects on multipole contributions and angular dependence in core-level spectroscopies
| العنوان: | Assessing temperature effects on multipole contributions and angular dependence in core-level spectroscopies |
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| المؤلفون: | Sean P. Collins, Ch. Brouder, Delphine Cabaret, Ch. J. Sahle, Guillaume Radtke, S. Delhommaye, Lorenzo Paulatto, Michele Lazzeri, Simo Huotari |
| المساهمون: | Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Diamond Light Source Ltd, University of Helsinki, European Synchrotron Radiation Facility (ESRF), Helsingin yliopisto = Helsingfors universitet = University of Helsinki, Helsinki In Vivo Animal Imaging Platform (HAIP), Department of Physics |
| المصدر: | Physical Review B Physical Review B, American Physical Society, 2021, 104 (2), ⟨10.1103/PhysRevB.104.024302⟩ Physical Review B, 2021, 104 (2), ⟨10.1103/PhysRevB.104.024302⟩ |
| بيانات النشر: | HAL CCSD, 2021. |
| سنة النشر: | 2021 |
| مصطلحات موضوعية: | TI-K-EDGE, RAMAN-SCATTERING, Thermal fluctuations, 02 engineering and technology, 01 natural sciences, 114 Physical sciences, Spectral line, LIGHT-ELEMENTS, 0103 physical sciences, SPECTRA, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], 010306 general physics, Physics, X-ray absorption spectroscopy, Valence (chemistry), RUTILE, IN-SITU, 021001 nanoscience & nanotechnology, XANES, Dipole, ELECTRONIC-STRUCTURE, X-RAY-ABSORPTION, Quadrupole, Density functional theory, Atomic physics, 0210 nano-technology, Multipole expansion, TRANSITION |
| الوصف: | This study aims at assessing the thermal nuclei motion effects on the multipole transition channels involved in two core-level spectroscopies, x-ray absorption spectroscopy (XAS) and x-ray Raman scattering (XRS). Temperature effects on the $1s\ensuremath{\rightarrow}s$ monopole, $1s\ensuremath{\rightarrow}p$ dipole, and $1s\ensuremath{\rightarrow}d$ quadrupole transitions are investigated using two reference systems for which we present original experimental data: $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{Al}}_{2}{\mathrm{O}}_{3}$ at the Al $K$ edge probed by XRS at room temperature and rutile $\mathrm{Ti}{\mathrm{O}}_{2}$ at the Ti $K$ pre-edge probed by XAS at temperatures ranging from 6 to 700 K. Through the latter, this work enlightens the part of the pre-edge peak enhancement due to temperature in the $K$ pre-edge region of $3d$ transition metal, which is known to be routinely used to determine the concentration, valence or symmetry of the probed element in a given sample. Nuclear thermal fluctuations are taken into account using a method based on density functional theory that consists in averaging spectra over atomic configurations, generated within the harmonic approximation and obeying quantum statistics at finite temperature. Since only a finite number of such configurations are used, the numerically averaged spectra generally lose the symmetry of the equilibrium crystal positions. In this paper, we demonstrate that the physical average has to be symmetric and propose a method to restore the physical angular dependence of the spectra. The approach is successfully applied to investigate the angular dependent XAS spectra in rutile as a function of temperature. The two systems under study allow to draw general conclusions regarding the effect of nuclear quantum fluctuations on the different transition channels available to both core-level spectroscopies. |
| اللغة: | English |
| تدمد: | 2469-9950 2469-9969 |
| URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::cd83790f11bd4460204f9d8e60d9faa8 https://hal.archives-ouvertes.fr/hal-03365381 |
| حقوق: | OPEN |
| رقم الأكسشن: | edsair.doi.dedup.....cd83790f11bd4460204f9d8e60d9faa8 |
| قاعدة البيانات: | OpenAIRE |
| تدمد: | 24699950 24699969 |
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