Electronic structure and core-level spectra of light actinide dioxides in the dynamical mean-field theory
Electronic structure and core-level spectra of light actinide dioxides in the dynamical mean-field theory
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DOI：
10.1103/physrevb.92.085125
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发表时间：
2015-08-17
影响因子：
3.7
通讯作者：
Lichtenstein, Alexander I.
中科院分区：
文献类型：
--
作者：
Kolorenc, Jindrich;Shick, Alexander B.;Lichtenstein, Alexander I.
将局部密度近似与动态平均场理论（LDA + DMFT）相结合，应用于光锕系二氧化物UO2、NpO2和PuO2的顺磁相。计算得到的带隙和价带电子结构与光吸收实验和光发射光谱吻合得很好。锕系元素的5f层与氧的2p层的杂化比较大；它增加了5f轨道的填充，从两个、三个和四个电子的名义离子构型到接近半整数的值2.5、3.4和4.4。这种大的杂化作用也在核能级的光发射光谱上留下了卫星峰的印记。结果表明，LDA + DMFT计算能准确再现这些卫星。
The local-density approximation combined with the dynamical mean-field theory (LDA + DMFT) is applied to the paramagnetic phase of light actinide dioxides: UO2, NpO2, and PuO2. The calculated band gaps and the valence-band electronic structure are in very good agreement with the optical absorption experiments as well as with the photoemission spectra. The hybridization of the actinide 5f shell with the 2p states of oxygen is found to be relatively large; it increases the filling of the 5f orbitals from the nominal ionic configurations with two, three, and four electrons to nearly half-integer values 2.5, 3.4, and 4.4. The large hybridization leaves an imprint also on the core-level photoemission spectra in the form of satellite peaks. It is demonstrated that these satellites are accurately reproduced by the LDA + DMFT calculations.