Microscopic investigation of enhanced Pauli paramagnetism in metallic Pu2C3

R. Yamamoto; M. S. Cook; A. R. Altenhof; P. Sherpa; S. Park; J. D. Thompson; H. E. Mason; D. C. Arellano; D. V. Prada; P. H. Tobash; F. Ronning; E. D. Bauer; N. Harrison; W. A. Phelan; A. P. Dioguardi; M. Hirata

doi:10.1103/n911-574l

Microscopic investigation of enhanced Pauli paramagnetism in metallic Pu₂C₃

R. Yamamoto
, M. S. Cook
, A. R. Altenhof
, P. Sherpa
, S. Park
, J. D. Thompson
, H. E. Mason
, D. C. Arellano
, D. V. Prada
, P. H. Tobash
, F. Ronning
, E. D. Bauer
, N. Harrison
, W. A. Phelan
, A. P. Dioguardi
, M. Hirata

Correlated Electron Materials

Research output: Contribution to journal › Article › peer-review

Abstract

A combined study of the structural and electronic properties of polycrystalline Pu₂C₃ is reported based on x-ray diffraction, specific heat, magnetic susceptibility, and ¹³C nuclear magnetic resonance (NMR). X-ray diffraction reveals a global noncentrosymmetric cubic lattice, with a nearest-neighbor C–C bond length of r = 1.38 Å. ¹³C NMR measurements indicate that the global cubic symmetry is locally broken, revealing two unique carbon environments. Magnetic susceptibility suggests enhanced Pauli paramagnetism, and specific heat reveals a moderately large electronic Sommerfeld coefficient γ = 45 mJ mol⁻ _Pu ¹ K⁻², with a Wilson ratio R_W ≈ 1.3 further indicating moderate correlations. ¹³C nuclear spin-lattice relaxation rate (1/T₁) and Knight shift (K) measurements find metallic Korringa behavior (i.e., T₁TK² = const.) with modest ferromagnetic spin fluctuations at low temperature. Taken together, the data point to a delocalized nature of a narrow 5 f-electron band with electronic correlations. Our data provide prime evidence for a plutonium-based metallic system with electronic correlations, which sheds new light on the understanding of complex paramagnetism in actinide-based metallic compounds.

Original language	English
Article number	165105
Pages (from-to)	1-10
Number of pages	10
Journal	Physical Review B
Volume	112
Issue number	16
DOIs	https://doi.org/10.1103/n911-574l
State	Published - Oct 3 2025

Funding

Crystal growth and NMR measurements were supported by the U.S. Department of Energy, Office of Basic Energy Sciences “Quantum Fluctuations in Narrow Band Systems” program. Thermodynamic measurements were supported by the Laboratory Directed Research and Development program.

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Yamamoto, R., Cook, M. S., Altenhof, A. R., Sherpa, P., Park, S., Thompson, J. D., Mason, H. E., Arellano, D. C., Prada, D. V., Tobash, P. H., Ronning, F., Bauer, E. D., Harrison, N., Phelan, W. A., Dioguardi, A. P., & Hirata, M. (2025). Microscopic investigation of enhanced Pauli paramagnetism in metallic Pu₂C₃. Physical Review B, 112(16), 1-10. Article 165105. https://doi.org/10.1103/n911-574l

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title = "Microscopic investigation of enhanced Pauli paramagnetism in metallic Pu2C3",

abstract = "A combined study of the structural and electronic properties of polycrystalline Pu2C3 is reported based on x-ray diffraction, specific heat, magnetic susceptibility, and 13C nuclear magnetic resonance (NMR). X-ray diffraction reveals a global noncentrosymmetric cubic lattice, with a nearest-neighbor C–C bond length of r = 1.38 {\AA}. 13C NMR measurements indicate that the global cubic symmetry is locally broken, revealing two unique carbon environments. Magnetic susceptibility suggests enhanced Pauli paramagnetism, and specific heat reveals a moderately large electronic Sommerfeld coefficient γ = 45 mJ mol− Pu 1 K−2, with a Wilson ratio RW ≈ 1.3 further indicating moderate correlations. 13C nuclear spin-lattice relaxation rate (1/T1) and Knight shift (K) measurements find metallic Korringa behavior (i.e., T1TK2 = const.) with modest ferromagnetic spin fluctuations at low temperature. Taken together, the data point to a delocalized nature of a narrow 5 f-electron band with electronic correlations. Our data provide prime evidence for a plutonium-based metallic system with electronic correlations, which sheds new light on the understanding of complex paramagnetism in actinide-based metallic compounds.",

author = "R. Yamamoto and Cook, \{M. S.\} and Altenhof, \{A. R.\} and P. Sherpa and S. Park and Thompson, \{J. D.\} and Mason, \{H. E.\} and Arellano, \{D. C.\} and Prada, \{D. V.\} and Tobash, \{P. H.\} and F. Ronning and Bauer, \{E. D.\} and N. Harrison and Phelan, \{W. A.\} and Dioguardi, \{A. P.\} and M. Hirata",

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AU - Yamamoto, R.

AU - Cook, M. S.

AU - Altenhof, A. R.

AU - Sherpa, P.

AU - Park, S.

AU - Thompson, J. D.

AU - Mason, H. E.

AU - Arellano, D. C.

AU - Prada, D. V.

AU - Tobash, P. H.

AU - Ronning, F.

AU - Bauer, E. D.

AU - Harrison, N.

AU - Phelan, W. A.

AU - Dioguardi, A. P.

AU - Hirata, M.

PY - 2025/10/3

Y1 - 2025/10/3

N2 - A combined study of the structural and electronic properties of polycrystalline Pu2C3 is reported based on x-ray diffraction, specific heat, magnetic susceptibility, and 13C nuclear magnetic resonance (NMR). X-ray diffraction reveals a global noncentrosymmetric cubic lattice, with a nearest-neighbor C–C bond length of r = 1.38 Å. 13C NMR measurements indicate that the global cubic symmetry is locally broken, revealing two unique carbon environments. Magnetic susceptibility suggests enhanced Pauli paramagnetism, and specific heat reveals a moderately large electronic Sommerfeld coefficient γ = 45 mJ mol− Pu 1 K−2, with a Wilson ratio RW ≈ 1.3 further indicating moderate correlations. 13C nuclear spin-lattice relaxation rate (1/T1) and Knight shift (K) measurements find metallic Korringa behavior (i.e., T1TK2 = const.) with modest ferromagnetic spin fluctuations at low temperature. Taken together, the data point to a delocalized nature of a narrow 5 f-electron band with electronic correlations. Our data provide prime evidence for a plutonium-based metallic system with electronic correlations, which sheds new light on the understanding of complex paramagnetism in actinide-based metallic compounds.

AB - A combined study of the structural and electronic properties of polycrystalline Pu2C3 is reported based on x-ray diffraction, specific heat, magnetic susceptibility, and 13C nuclear magnetic resonance (NMR). X-ray diffraction reveals a global noncentrosymmetric cubic lattice, with a nearest-neighbor C–C bond length of r = 1.38 Å. 13C NMR measurements indicate that the global cubic symmetry is locally broken, revealing two unique carbon environments. Magnetic susceptibility suggests enhanced Pauli paramagnetism, and specific heat reveals a moderately large electronic Sommerfeld coefficient γ = 45 mJ mol− Pu 1 K−2, with a Wilson ratio RW ≈ 1.3 further indicating moderate correlations. 13C nuclear spin-lattice relaxation rate (1/T1) and Knight shift (K) measurements find metallic Korringa behavior (i.e., T1TK2 = const.) with modest ferromagnetic spin fluctuations at low temperature. Taken together, the data point to a delocalized nature of a narrow 5 f-electron band with electronic correlations. Our data provide prime evidence for a plutonium-based metallic system with electronic correlations, which sheds new light on the understanding of complex paramagnetism in actinide-based metallic compounds.

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JO - Physical Review B

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Microscopic investigation of enhanced Pauli paramagnetism in metallic Pu₂C₃

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