First-principles calculation of the Coulomb interaction parameters U and J for actinide dioxides
| Autor: | Bernard Amadon, Robinson Outerovitch, Jean Baptiste Morée |
|---|---|
| Rok vydání: | 2021 |
| Předmět: |
Physics
Wannier function 02 engineering and technology 021001 nanoscience & nanotechnology Coupling (probability) 01 natural sciences Atomic orbital Ab initio quantum chemistry methods Quantum mechanics 0103 physical sciences Density of states Coulomb Antiferromagnetism 010306 general physics 0210 nano-technology Random phase approximation |
| Zdroj: | Physical Review B. 103 |
| ISSN: | 2469-9969 2469-9950 |
| DOI: | 10.1103/physrevb.103.045113 |
| Popis: | We present ab initio calculations of effective interaction parameters $U$ and $J$ for dioxides of actinides from uranium to curium. We first use a self-consistent scheme using $\mathrm{DFT}+U$ and constrained random phase approximation (cRPA). For ${\mathrm{UO}}_{2}$, and ${\mathrm{NpO}}_{2}$, we find self-consistent values of $U$ and $J$ leading to values of gap in agreement with experiments. For ${\mathrm{PuO}}_{2}$, the value of $U$ is underestimated. For ${\mathrm{AmO}}_{2}$ and ${\mathrm{CmO}}_{2}$, we find very low self-consistent values. We compare projected local orbital Wannier functions to maximally localized Wannier functions and find a weak effect of the localization on interaction parameters. We suggest that spin-orbit coupling, and antiferromagnetism, could improve these results partially. We also extend our calculations by treating the $p$ bands from oxygen as correlated, as in Seth et al. [Phys. Rev. Lett. 119, 056401 (2017)], and show that the results are rather independent of self-consistency in this approach. Comparing these calculations, our conclusion is that including electron interaction on oxygen $p$ orbitals is necessary both to improve the density of states and to compute more meaningful and predictive values of effective interaction parameters. |
| Databáze: | OpenAIRE |
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