The Valence-Fluctuating Ground State of Plutonium

Abstract

A central issue in material science is to obtain understanding of the electronic correlations that control complex materials. Such electronic correlations frequently arise due to the competition of localized and itinerant electronic degrees of freedom. While the respective limits of well-localized or entirely itinerant ground states are well-understood, the intermediate regime that controls the functional properties of complex materials continues to challenge theoretical understanding. We have used neutron spectroscopy to investigate plutonium, which is a prototypical material at the brink between bonding and non-bonding configurations. Our study reveals that the ground state of plutonium is governed by valence fluctuations, that is, a quantum-mechanical superposition of localized and itinerant electronic configurations as recently predicted by dynamical mean field theory. Our results not only resolve the long-standing controversy between experiment and theory on plutonium's magnetism, but also suggest an improved understanding of the effects of such electronic dichotomy in complex materials.

29 pages, 2 figures, 2 tables, supplementary materials

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Cited by in corpus (30)

• Metal-insulator Transition in VO2: a DFT+DMFT perspective
• Thermal Energy Transport in Oxide Nuclear Fuel
• Topological magnon band structure of emergent Landau levels in a skyrmion lattice
• Nature of the 5$f$ electronic structure of plutonium
• Emergence of quantum critical charge and spin-state fluctuations near the pressure-induced Mott transition in MnO, FeO, CoO, and NiO
• Ultra-High Resolution Neutron Spectroscopy of Low-Energy Spin Dynamics in UGe${}_2$
• Unconventional Hund Metal in a Weak Itinerant Ferromagnet
• Advances in actinide thin films: synthesis, properties, and future directions
• Emergence of quasiparticle multiplets in curium
• Uncovering the Origin of Divergence in the CsM(CrO${}_4$)${}_2$ (M = La, Pr, Nd, Sm, Eu; Am) Family through Examination of the Chemical Bonding in a Molecular Cluster and by Band Structure Analysis
• Electronic Correlation Induced Expansion of Compensated Electron and Hole Fermi Pockets in delta-Plutonium
• Low temperature magnetic structure of CeRhIn${}_5$ by neutron diffraction on absorption-optimized samples
• Pressure-Driven 5$f$ Localized-Itinerant Transition and Valence Fluctuation in Californium
• Correlation strength and orbital differentiation across the phase diagram of plutonium metal
• Isochronal annealing effects on local structure, crystalline fraction, and undamaged region size of radiation damage in Ga-stabilized $\delta$-Pu
• Phase stabilization by electronic entropy in plutonium
• ${}^{239}$Pu nuclear magnetic resonance in the candidate topological insulator PuB${}_4$
• Site and orbital selective correlations in $\beta$-Pu
• Orbital-dependent correlations in PuCoGa${}_5$
• Phase transitions and spin-state of iron in FeO at the conditions of Earth's deep interior
• Temperature-driven hidden 5f itinerant-localized crossover in heavy-fermion compound PuIn3
• Electronic correlations of element cerium under high pressure
• Collapse of quasiparticle multiplets and $5f$ itinerant-localized crossovers in cubic phase Pu${}_3$Ga
• Extended Nuclear Quadrupole Resonance Study of the Heavy-Fermion Superconductor PuCoGa${}_5$
• Charge self-consistent density functional theory plus ghost rotationally-invariant slave-boson theory for correlated materials
• Neutron scattering off Weyl semimetals
• Electronically driven collapse of the bulk modulus in $\delta$-plutonium
• Local aging effects in PuB${}_4$: Growing inhomogeneity and slow dynamics of local-field fluctuations probed by ${}^{239}$Pu NMR
• Reexaming the ground state and magnetic properties of curium dioxide
• Microscopic investigation of enhanced Pauli paramagnetism in metallic Pu${}_2$C${}_3$