TY - JOUR

T1 - First-principles calculation of the Coulomb interaction parameters U and J for actinide dioxides

AU - Morée, Jean Baptiste

AU - Outerovitch, Robinson

AU - Amadon, Bernard

N1 - Publisher Copyright:
© 2021 American Physical Society.

PY - 2021/1/11

Y1 - 2021/1/11

N2 - 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 DFT+U and constrained random phase approximation (cRPA). For UO2, and NpO2, we find self-consistent values of U and J leading to values of gap in agreement with experiments. For PuO2, the value of U is underestimated. For AmO2 and CmO2, 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)PRLTAO0031-900710.1103/PhysRevLett.119.056401], 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.

AB - 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 DFT+U and constrained random phase approximation (cRPA). For UO2, and NpO2, we find self-consistent values of U and J leading to values of gap in agreement with experiments. For PuO2, the value of U is underestimated. For AmO2 and CmO2, 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)PRLTAO0031-900710.1103/PhysRevLett.119.056401], 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.

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U2 - 10.1103/PhysRevB.103.045113

DO - 10.1103/PhysRevB.103.045113

M3 - Article

AN - SCOPUS:85099282524

VL - 103

JO - Physical Review B-Condensed Matter

JF - Physical Review B-Condensed Matter

SN - 2469-9950

IS - 4

M1 - 045113

ER -