Shick Alexander B, Wdowik Urszula D, Halevy Itzhak, Legut Dominik
Institute of Physics, Czech Academy of Science, Na Slovance 2, 18221, Prague, Czech Republic.
Department of Molecular Chemistry and Materials Science, Weizmann Institute of Science, Rehovoth, 76100, Israel.
Sci Rep. 2024 Oct 25;14(1):25337. doi: 10.1038/s41598-024-75321-4.
Correlated band theory implemented as a combination of the relativistic density functional theory with exact diagonalization [DFT+U(ED)] of the Anderson impurity term with Coulomb repulsion U in the 5f shell is applied to the magnetic field polarized state of [Formula: see text]. We demonstrate that the DFT+U(ED) approach provides a good agreement with very recent x-ray absorbtion near edge structure (XANES) and x-ray magnetic circular dichroism (XMCD) experiments. The branching ratio for the [Formula: see text] edge transitions of uranium, and the valence spin-orbit interaction per hole were evaluated in a perfect agreement with the XANES. The orbital-to-spin moment ratio is calculated with DFT+U(ED) within the range of values extracted from XMCD data. The uranium atom 5f-shell ground state with 33 % of [Formula: see text] and 58 % of [Formula: see text] configurations is determined. Both XMCD and DFT+U(ED) point out the intermediate valence of uranium as well as itinerant-localized dichotomy in [Formula: see text].
将相对论密度泛函理论与5f壳层中具有库仑排斥力U的安德森杂质项的精确对角化[DFT + U(ED)]相结合实现的关联能带理论，应用于[公式：见正文]的磁场极化态。我们证明，DFT + U(ED)方法与非常新的x射线吸收近边结构（XANES）和x射线磁圆二色性（XMCD）实验结果吻合良好。对铀的[公式：见正文]边跃迁的分支比以及每个空穴的价态自旋 - 轨道相互作用进行了评估，结果与XANES完全一致。利用DFT + U(ED)在从XMCD数据提取的值的范围内计算了轨道磁矩与自旋磁矩之比。确定了铀原子5f壳层基态具有33%的[公式：见正文]和58%的[公式：见正文]构型。XMCD和DFT + U(ED)都指出了铀的中间价态以及[公式：见正文]中的巡游 - 局域二分法。
