Academic Journal
Electronic structure and bonding properties of U6+ by high-resolution X-ray spectroscopy and computations
| العنوان: | Electronic structure and bonding properties of U6+ by high-resolution X-ray spectroscopy and computations |
|---|---|
| المؤلفون: | Ramanantoanina, Harry, Neil, T., Palina, Natalia, Schacherl, Bianca, Prüßmann, Tim, Hauschild, D., Steiniger, R., Heske, C., Weinhardt, L., Haverkort, M., Vitova, Tonya |
| سنة النشر: | 2024 |
| المجموعة: | KITopen (Karlsruhe Institute of Technologie) |
| مصطلحات موضوعية: | ddc:600, Technology, info:eu-repo/classification/ddc/600 |
| الوصف: | Understanding the chemistry of actinide compounds is crucial in many fields including medical research, energy, and radioactive materials disposal, and accordingly a number of in-depth studies have been conducted. [1] However, the electronic structures and bonding properties of actinides have not been studied as deeply as those for lanthanides or transition metals. In this work, we describe the use of high-energy resolution X-ray absorption/emission spectroscopy (HR-XAS and HR-XES, respectively) and resonant inelastic X-ray scattering (RIXS) techniques to probe the local atomic and electronic structures of the molecular [(UO2)F5] 3-, [(UO2)Cl4] 2-, and [(UO2)Br4] 2- complexes. In addition, we also detail the methodological approach for predicting the ligand K-edge high-energy resolution XANES, and U M4,5-edge core-to-core/valence band RIXS by means of first principles density-functional theory (DFT) calculations by using a time-dependent formalism and multiplet calculations, respectively, at the relativistic level (4-component Dirac Hamiltonian). [2] By comparing the theoretical and experimental spectra, our study also provides insight into the roles of the uranium 5f and 6d orbitals for the metal ligand bonding as a function of the equatorial ligand (fluoride, chloride, and bromide). The X-ray spectroscopic experiments were performed at the Karlsruher Research Accelerator (KARA) Light Source (Karlsruhe, Germany). The U M4-edge and Br K-edge high energy resolution X-ray absorption emission and resonant inelastic X-ray scattering data were recorded at the ACT station of the CAT-ACT beamline, [3a] the Cl K-edge XANES at the INE-Beamline, [3b] and the F K-edge XANES at the X-SPEC beamline. [3c] This work is supported by the ERC Consolidator grant “the Actinide Bond” (N° 101003292) under the European Union’s Horizon 2020 research and innovation program. [1] (a) Tobin, J.G.; Ramanantoanina, H.; Daul, C.; Poussel, P.; Yu, S.-W.; Nowak, S.; Alonso-Mori, R.; Kroll, T.; Nordlund, D.; Weng, T.-C.; Sokaras, D.; Phys. Rev. ... |
| نوع الوثيقة: | article in journal/newspaper conference object |
| اللغة: | English |
| Relation: | https://publikationen.bibliothek.kit.edu/1000168394 |
| الاتاحة: | https://publikationen.bibliothek.kit.edu/1000168394 |
| رقم الانضمام: | edsbas.D330B7C2 |
| قاعدة البيانات: | BASE |
| الوصف غير متاح. |