Autor: |
C. L. Silva, L. Amidani, M. Retegan, S. Weiss, E. F. Bazarkina, T. Graubner, F. Kraus, K. O. Kvashnina |
Jazyk: |
angličtina |
Rok vydání: |
2024 |
Předmět: |
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Zdroj: |
Nature Communications, Vol 15, Iss 1, Pp 1-10 (2024) |
Druh dokumentu: |
article |
ISSN: |
2041-1723 |
DOI: |
10.1038/s41467-024-50924-7 |
Popis: |
Abstract The significant interest in actinide bonding has recently focused on novel compounds with exotic oxidation states. However, the difficulty in obtaining relevant high-quality experimental data, particularly for low-valent actinide compounds, prevents a deeper understanding of 5f systems. Here we show X-ray absorption near-edge structure (XANES) measurements in the high-energy resolution fluorescence detection (HERFD) mode at the uranium M4 edge for the UIII and UIV halides, namely UX3 and UX4 (X = F, Cl, Br, I). The spectral shapes of these two series exhibit clear differences, which we explain using electronic structure calculations of the 3d-4f resonant inelastic X-ray scattering (RIXS) process. To understand the changes observed, we implemented crystal field models with ab initio derived parameters and investigated the effect of reducing different contributions to the electron-electron interactions involved in the RIXS process. Our analysis shows that the electron-electron interactions weaken as the ligand changes from I to F, indicative of a decrease in ionicity both along and between the UX3 and UX4 halide series. |
Databáze: |
Directory of Open Access Journals |
Externí odkaz: |
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