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Magnetic order and valence fluctuation in a PuGa intermetallic compound studied via a first principles calculation
Author(s) -
Li Rusong,
Lu Xing,
Xin Duqiang,
Wang Jintao,
Ao Bingyun
Publication year - 2020
Publication title -
international journal of quantum chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.484
H-Index - 105
eISSN - 1097-461X
pISSN - 0020-7608
DOI - 10.1002/qua.26105
Subject(s) - density functional theory , intermetallic , antiferromagnetism , condensed matter physics , electronic structure , valence (chemistry) , chemistry , magnetism , physics , alloy , computational chemistry , quantum mechanics , organic chemistry
In order to reveal electronic properties of a plutonium‐gallium intermetallic compound (Pu 3 Ga), and its potential implication for microscopic mechanisms for effects of Ga doping on the electronic and structural properties, as well as the phase stability of delta‐phase PuGa alloy, a first principles calculation on the magnetic properties of this system is implemented by using density functional theory (DFT) plus on‐site Coulomb repulsion U with nonmagnetic, ferromagnetic, and antiferromagnetic (AFM) orders, while the intermediate correlation effect, which is beyond the scope of pure itinerant and localized electronic model, is investigated by using a many‐body technique combining DFT and dynamical mean‐field theory considering the dynamical correlation effect due to the incompletely filled Pu 5 f orbitals and the relativistic effect by inclusion of spin‐orbit coupling (SOC). Our findings show that Pu 3 Ga is a bad metal with AFM order, which is in good agreement with the experimental magnetic measurement. SOC further splitting Pu 5 f states into j = 5/2 and j = 7/2 manifolds, the former exhibits metallic character, while the latter insulating feature. Occupation analysis establishes that an average occupancy of Pu 5 f electrons in Pu 3 Ga is n f = 4.9598, this result together with the spectrum function indicates that 5 f electrons in this system might be a localized state with strong valence fluctuation. Additionally, optimization of lattice parameter, density of state, and momentum‐resolved electronic spectrum function are also presented.