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DOE OSTI · 2572568

Experimental and Theoretical Confirmation of Covalent Bonding in α‐Pu

Muñoz, Alexander Reed [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000169653753)·Cook, Matthew Scott [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000288777505)·Arellano, David Carl [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000253977216)·Abeykoon, AM Milinda [Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000169653753)·Mitchell, Jeremy Neil [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000171093505)·Hernandez, Sarah Christine [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:000000021432700X)·Bauer, Eric Dietzgen [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000300171937)·Mizzi, Christopher Adam [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:000000024209854X)·Maiorov, Boris Alfredo [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000318850436)·Harrison, Neil [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000154567756)·Phelan, William Adam [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000187871965)
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Abstract

Plutonium's radioactivity provides functionality for nuclear batteries, nuclear reactors, etc., but its complex electronic properties harbor strongly correlated behavior giving rise to a host of interesting phenomena including the presence of a ca. 25% volume collapse between δ-Pu and α-Pu. The complex bonding environments of the ground state allotrope, α-Pu, serve as a unique testing ground for new computational and experimental approaches within the Pu science community. For the first time, a combination of novel ansatzes is used in all-electron density functional theory (DFT) and pair distribution functions (PDF) obtained from high-Q X-ray diffraction to study the bonding behavior in α-Pu. This first experimental and theoretical co-informed description of local bonding behavior for α-Pu reveals covalent bonds, which is a topic that remains of interest in this allotrope. The covalent bonding present at the atomistic level accounts for several of α-Pu's macropscopic properties (e.g., Poisson's ratio) that in turn explains its physical functionalities relative to other allotropic phases like δ-Pu.

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36 MATERIALS SCIENCE37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITYDFT calculationsbondingpair distribution functionplutoniumquantum theory of atoms in molecules

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Muñoz, Alexander Reed [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000169653753), Cook, Matthew Scott [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000288777505), Arellano, David Carl [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000253977216), Abeykoon, AM Milinda [Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000169653753), Mitchell, Jeremy Neil [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000171093505), Hernandez, Sarah Christine [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:000000021432700X), Bauer, Eric Dietzgen [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000300171937), Mizzi, Christopher Adam [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:000000024209854X), Maiorov, Boris Alfredo [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000318850436), Harrison, Neil [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000154567756), Phelan, William Adam [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000187871965). 2025-06-29. Experimental and Theoretical Confirmation of Covalent Bonding in α‐Pu. https://doi.org/10.1002/adfm.202501798

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