Temperature-driven emergence of local moment in <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mi>δ</mml:mi> </mml:math> -plutonium

In this work, the electronic structure, the uniform magnetic susceptibility, and the static and dynamic local magnetic susceptibilities of $\ensuremath{\delta}$-Pu are investigated with the help of density functional theory (DFT) plus dynamical mean-field theory. Consistent with experimental observations and at variance with DFT, the ground state at low temperature is found to be nonmagnetic and characterized as a mixed-valence system, where the local magnetic moment from the partially filled $5f$ shell is effectively screened by the conduction electrons. Importantly, as the temperature rises a local magnetic moment emerges with antiparallel orbital and spin angular momenta, leading to a transition from a Pauli-like behavior to an apparent weak Curie-Weiss magnetism in the uniform magnetic susceptibility. The crossover regime corresponds to the emergence of a local moment as evidenced by the local susceptibilities. This finding reconciles previous discrepancies between experimental observation and theoretical simulations.

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Publication Details

Journal
Physical review. B./Physical review. B
Published
2025-09-26
DOI
https://doi.org/10.1103/28p8-l3pd
Primary Topic
Rare-earth and actinide compounds
Type
article
Field-Weighted Citation Impact
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article

Temperature-driven emergence of local moment in <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mi>δ</mml:mi> </mml:math> -plutonium

Bernard Amadon, Frédéric Gendron
Physical review. B./Physical review. B
Rare-earth and actinide compounds
article

Temperature-driven emergence of local moment in <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mi>δ</mml:mi> </mml:math> -plutonium

Bernard Amadon, Frédéric Gendron
article en

Abstract

In this work, the electronic structure, the uniform magnetic susceptibility, and the static and dynamic local magnetic susceptibilities of $\ensuremath{\delta}$-Pu are investigated with the help of density functional theory (DFT) plus dynamical mean-field theory. Consistent with experimental observations and at variance with DFT, the ground state at low temperature is found to be nonmagnetic and characterized as a mixed-valence system, where the local magnetic moment from the partially filled $5f$ shell is effectively screened by the conduction electrons. Importantly, as the temperature rises a local magnetic moment emerges with antiparallel orbital and spin angular momenta, leading to a transition from a Pauli-like behavior to an apparent weak Curie-Weiss magnetism in the uniform magnetic susceptibility. The crossover regime corresponds to the emergence of a local moment as evidenced by the local susceptibilities. This finding reconciles previous discrepancies between experimental observation and theoretical simulations.

Physical review. B./Physical review. BVol. 112(14)
Commissariat à l'Énergie Atomique et aux Énergies Alternatives (FR), Université Paris-Saclay (FR), CEA DAM Île-de-France (FR)
Openalex Percentile: Top 81%
Rare-earth and actinide compounds
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