Microscopic investigation of enhanced Pauli paramagnetism in metallic Pu$_2$C$_3$

Fuente: arXiv
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Auteurs principaux: 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.
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Publié: 2025
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author 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.
author_facet 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.
contents A combined study of the structural and electronic properties of polycrystalline Pu$_2$C$_3$ is reported based on x-ray diffraction, specific heat, magnetic susceptibility, ${}^{13}$C nuclear magnetic resonance (NMR), and band structure calculations. X-ray diffraction reveals a global noncentrosymmetric cubic lattice, with a nearest-neighbor C--C bond length of $r = 1.38$ Å. ${}^{13}$C 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$_{\mathrm{Pu}}^{-1}$ K$^{-2}$, with a Wilson ratio $R_W \approx 1.3$ further indicating moderate correlations. ${}^{13}$C nuclear spin-lattice relaxation rate ($1/T_1$) and Knight shift ($K$) measurements find metallic Korringa behavior (i.e., $T_1TK^2=$ 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 weak electronic correlations. Density functional theory band-structure calculations confirm the appearance of such narrow 5$f$ bands near the Fermi level. Our data provide prime evidence for a plutonium-based metallic system with weak electronic correlations, which sheds new light on the understanding of complex paramagnetism in actinide-based metallic compounds.
format Preprint
id arxiv_https___arxiv_org_abs_2506_09911
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Microscopic investigation of enhanced Pauli paramagnetism in metallic Pu$_2$C$_3$
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.
Strongly Correlated Electrons
A combined study of the structural and electronic properties of polycrystalline Pu$_2$C$_3$ is reported based on x-ray diffraction, specific heat, magnetic susceptibility, ${}^{13}$C nuclear magnetic resonance (NMR), and band structure calculations. X-ray diffraction reveals a global noncentrosymmetric cubic lattice, with a nearest-neighbor C--C bond length of $r = 1.38$ Å. ${}^{13}$C 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$_{\mathrm{Pu}}^{-1}$ K$^{-2}$, with a Wilson ratio $R_W \approx 1.3$ further indicating moderate correlations. ${}^{13}$C nuclear spin-lattice relaxation rate ($1/T_1$) and Knight shift ($K$) measurements find metallic Korringa behavior (i.e., $T_1TK^2=$ 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 weak electronic correlations. Density functional theory band-structure calculations confirm the appearance of such narrow 5$f$ bands near the Fermi level. Our data provide prime evidence for a plutonium-based metallic system with weak electronic correlations, which sheds new light on the understanding of complex paramagnetism in actinide-based metallic compounds.
title Microscopic investigation of enhanced Pauli paramagnetism in metallic Pu$_2$C$_3$
topic Strongly Correlated Electrons
url https://arxiv.org/abs/2506.09911