arXiv subjects

P. H. Tobash

Publications and source records attributed to P. H. Tobash.

At least 19 recordsLinked to original sources

arXiv2025

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

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.

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arXiv2023

Nesting-driven antiferromagnetic order in Kondo lattice CePd5Al2

We investigated the electronic structure of the antiferromagnetic Kondo lattice CePd5Al2 using high-resolution angle-resolved photoemission spectroscopy. The experimentally determined band structure of the conduction electrons is predominated by the Pd 4d character. It contains multiple hole and electron Fermi pockets, in good agreement with density functional theory calculations. The Fermi surface is folded over Q0 = (0, 0, 1), manifested by Fermi surface reconstruction and band folding. Our results suggest that Fermi surface nesting drives the formation of antiferromagnetic order in CePd5Al2.

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arXiv2022

Pseudogap in elemental plutonium

Electronic correlations associated with incipient magnetism have long been recognized as an important factor in stabilizing the largest atomic volume $δ$ phase of plutonium, yet their strength compared to those in the rare earths and neighboring actinides in the Periodic Table has largely remained a mystery. We show here using calorimetry measurements, together with prior detailed measurements of the phonon dispersion, that the $5f$ electrons of the $δ$ phase reside in a pseudogapped state, accompanied by reductions in various physical properties below a characteristic temperature $T^\ast\approx$~100~K. The small characteristic energy scale of the pseudogapped state implies that the $5f$ electrons in plutonium are much closer to the threshold for localization and magnetic order than has been suggested by state-of-the-art electronic structure theory, revealing plutonium to be arguably the most strongly correlated of the elements.

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arXiv2019

Competing Electronic Configurations for PuTe and New Insight on Plutonium Metal

The electronic structure of plutonium metal and its compounds pose a grand challenge for a fundamental understanding of the Pu-5$f$ electron character. For 30 years the plutonium chalcogenides have been especially challenging, and multiple theoretical scenarios have been proposed to explain their unusual behavior. We present extensive high-resolution photoemission data on a single crystal of PuTe, which has also been proposed as a topological insulator. The new experimental results on this mixed-valent material provide a constraint to the theoretical modeling and new dynamical mean-field theory calculations agree with the experimental results. Comparisons with Pu metal provide new insight in understanding its complex electronic structure.

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arXiv2019

Phase stabilization by electronic entropy in plutonium

(Pu) has an unusually rich phase diagram that includes seven distinct solid state phases and an unusually large 25% collapse in volume from its delta phase to its low temperature alpha phase via a series of structural transitions. Despite considerable advances in our understanding of strong electronic correlations within various structural phases of Pu and other actinides, the thermodynamic mechanism responsible for driving the volume collapse has continued to remain a mystery. Here we utilize the unique sensitivity of magnetostriction measurements to unstable f electron shells to uncover the crucial role played by electronic entropy in stabilizing delta-Pu against volume collapse. We find that in contrast to valence fluctuating rare earths, which typically have a single f electron shell instability whose excitations drive the volume in a single direction in temperature and magnetic field, delta-Pu exhibits two such instabilities whose excitations drive the volume in opposite directions while producing an abundance of entropy at elevated temperatures. The two instabilities imply a near degeneracy between several different configurations of the 5f atomic shell, giving rise to a considerably richer behavior than found in rare earth metals. We use heat capacity measurements to establish a robust thermodynamic connection between the two excitation energies, the atomic volume, and the previously reported excess entropy of delta-Pu at elevated temperatures.

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arXiv2017

Hybridization gap in the heavy-fermion compound UPd$_2$Al$_3$ via quasiparticle scattering spectroscopy

We present results from point-contact spectroscopy of the antiferromagnetic heavy-fermion superconductor UPd$_2$Al$_3$: conductance spectra are taken from single crystals with two major surface orientations as a function of temperature and magnetic field, and analyzed using a theory of co-tunneling into an Anderson lattice. Spectroscopic signatures are clearly identified including the distinct asymmetric double-peak structure arising from the opening of a hybridization gap when a coherent heavy Fermi liquid is formed. Both the hybridization gap, found to be 7.2 $\pm$ 0.3 meV at 4 K, and the conductance enhancement above a flat background decrease upon increasing temperature. While the hybridization gap is extrapolated to remain finite up to $\sim$28 K, close to the temperature around which the magnetic susceptibility displays a broad peak, the conductance enhancement vanishes at $\sim$18 K, slightly above the antiferromagnetic transition temperature ($T_\textrm{N}$ $\approx$ 14 K). This rapid decrease of the conductance enhancement is understood as a consequence of the junction drifting away from the ballistic regime due to increased scattering off magnons associated with the localized U 5$f$ electrons. This shows that while the hybridization gap opening is not directly associated with the antiferromagnetic ordering, its visibility in the conductance is greatly affected by the temperature-dependent magnetic excitations. Our findings are not only consistent with the 5$f$ dual-nature picture in the literature but also shed new light on the interplay between the itinerant and localized electrons in UPd$_2$Al$_3$.

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arXiv2016

Extended Nuclear Quadrupole Resonance Study of the Heavy-Fermion Superconductor PuCoGa$_5$

PuCoGa$_5$ has emerged as a prototypical heavy-fermion superconductor, with its transition temperature ($T_c\simeq18.5$ K) being the highest amongst such materials. Nonetheless, a clear description as to what drives the superconducting pairing is still lacking, rendered complicated by the notoriously intricate nature of plutonium's 5$f$ valence electrons. Here, we present a detailed $^{69,71}$Ga nuclear quadrupole resonance (NQR) study of PuCoGa$_5$, concentrating on the system's normal state properties near to $T_c$ and aiming to detect distinct signatures of possible pairing mechanisms. In particular, the quadrupole frequency and spin-lattice relaxation rate were measured for the two crystallographically inequivalent Ga sites and for both Ga isotopes, in the temperature range 1.6 K - 300 K. No evidence of significant charge fluctuations is found from the NQR observables. On the contrary, the low-energy dynamics is dominated by anisotropic spin fluctuations with strong, nearly critical, in-plane character, which are effectively identical to the case of the sister compound PuCoIn$_5$. These findings are discussed within the context of different theoretical proposals for the unconventional pairing mechanism in heavy-fermion superconductors.

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arXiv2015

Determination of spin and orbital magnetization in the ferromagnetic superconductor UCoGe

The magnetism in the ferromagnetic superconductor UCoGe has been studied using a combination of magnetic Compton scattering, bulk magnetization, X-ray magnetic circular dichroism and electronic structure calculations, in order to determine the spin and orbital moments. The experimentally observed total spin moment, $M_s$, was found to be -0.24 $\pm$ 0.05~$μ_B$ at 5~T. By comparison with the total moment of 0.16 $\pm$ 0.01~$μ_B$, the orbital moment, $M_l$, was determined to be 0.40 $\pm$ 0.05~$μ_B$. The U and Co spin moments were determined to be antiparallel. We find that the U 5\textit{f} electrons carry a spin moment of U$_s \approx$ -0.30~$μ_B$ and that there is a Co spin moment of Co$_s \approx$ 0.06~$μ_B$ induced via hybridization. The ratio U$_l/$U$_s$, of $-1.3 \pm 0.3$, shows the U moment to be itinerant. In order to ensure an accurate description of the properties of 5\textit{f} systems, and to provide a critical test of the theoretical approaches, it is clearly necessary to obtain experimental data for both the spin and orbital moments, rather than just the total magnetic moment. This can be achieved simply by measuring the spin moment with magnetic Compton scattering and comparing this to the total moment from bulk magnetization.

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arXiv2015

Evidence for broken time-reversal symmetry in the superconducting phase of URu$_2$Si$_2$

Recent experimental and theoretical interest in the superconducting phase of the heavy fermion material URu$_2$Si$_2$ has led to a number of proposals in which the superconducting order parameter breaks time-reversal symmetry (TRS). In this study we measured polar Kerr effect (PKE) as a function of temperature for several high-quality single crystals of URu$_2$Si$_2$. We find an onset of PKE below the superconducting transition that is consistent with a TRS-breaking order parameter. This effect appears to be independent of an additional, possibly extrinsic, PKE generated above the hidden order transition at $T_{HO}=17.5$ K, and contains structure below $T_c$ suggestive of additional physics within the superconducting state.

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arXiv2014

Avoided Valence Transition in a Plutonium Superconductor

Some of the most remarkable phenomena---and greatest theoretical challenges---in condensed matter physics arise when $d$ or $f$ electrons are neither fully localized around their host nuclei, nor fully itinerant. This localized/itinerant "duality" underlies the correlated electronic states of the high-$T_c$ cuprate superconductors and the heavy-fermion intermetallics, and is nowhere more apparent than in the $5f$ valence electrons of plutonium. Here we report the full set of symmetry-resolved elastic moduli of $PuCoGa_5$---the highest $T_c$ superconductor of the heavy fermions ($T_c$=18.5 K)---and find that the bulk modulus softens anomalously over a wide range in temperature above $T_c$. Because the bulk modulus is known to couple strongly to the valence state, we propose that plutonium valence fluctuations drive this elastic softening. This elastic softening is observed to disappear when the superconducting gap opens at $T_c$, suggesting that plutonium valence fluctuations have a strong footprint on the Fermi surface, and that $PuCoGa_5$ avoids a valence-transition by entering the superconducting state. These measurements provide direct evidence of a valence instability in a plutonium compound, and suggest that the unusually high-$T_c$ in this system is driven by valence fluctuations.

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arXiv2014

Magnetic Order in the 2D Heavy-Fermion System CePt2In7 studied by muSR

The low-temperature microscopic magnetic properties of the quasi-2D heavyfermion compound, CePt2In7 are investigated by using a positive muon-spin rotation and relaxation (?muSR) technique. Clear evidence for the formation of a commensurate antiferromagnetic order below TN=5.40 K is presented. The magnetic order parameter is shown to fit well to a modified BSC gap-energy function in a strong-coupling scenario.

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arXiv2014

Microscopic Properties of the Heavy-Fermion Superconductor PuCoIn$_5$ Explored by Nuclear Quadrupole Resonance

We report $^{115}$In nuclear quadrupolar resonance (NQR) measurements on the heavy-fermion superconductor PuCoIn$_5$, in the temperature range $0.29{\rm K}\leq T\leq 75{\rm K}$. The NQR parameters for the two crystallographically inequivalent In sites are determined, and their temperature dependence is investigated. A linear shift of the quadrupolar frequency with lowering temperature below the critical value $T_c$ is revealed, in agreement with the prediction for composite pairing. The nuclear spin-lattice relaxation rate $T_1^{-1}(T)$ clearly signals a superconducting (SC) phase transition at $T_c\simeq 2.3$K, with strong spin fluctuations, mostly in-plane, dominating the relaxation process in the normal state near to $T_c$. Analysis of the $T_1^{-1}$ data in the SC state suggests that PuCoIn$_5$ is a strong-coupling $d$-wave superconductor.

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arXiv2013

Bulk evidence for a time reversal symmetry broken superconducting state in URu2Si2

URu$_2$Si$_2$ is claimed to be a chiral \emph{d}-wave superconductor with a $k_z (k_x \pm ik_y)$ time-reversal symmetry broken orbital component for the Cooper pair wave-function, which contains both nodal points and lines of nodes \cite{kasahara, kasahara2}. To study the magnetic response of such an unconventional state through a bulk, thermodynamic probe, we measured the magnetic torque $τ$ in very high-quality, well-characterized URu$_2$Si$_2$ single-crystals \cite{altarawneh,altarawneh2} at high magnetic-fields $H$ and at very low temperatures $T$. The magnetization $M(H) \propto τ(H) /H$ of URu$_2$Si$_2$, in its superconducting state and for angles within $15^{\circ}$ from the \emph{ab}-plane, reveals a change in its sign for $H$ approaching $H_{c2}$: from a clear diamagnetic response dominated by the pinning of vortices to a state with a smaller but "paramagnetic-like" hysteretic response which \emph{disappears} at $H_{c2}$, thus implying that it is intrinsically related to the superconducting state. We argue that this anomalous, angular-dependent behavior is evidence for a time-reversal symmetry broken superconducting state in URu$_2$Si$_2$, although not necessarily for the $k_z (k_x \pm ik_y)$ state.

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arXiv2013

Pressure phase diagram and quantum criticality of CePt2In7 single crystals

We report the temperature-pressure (T-P) phase diagram of CePt2In7 single crystals, especially the pressure evolution of the antiferromagnetic order and the emergence of superconductivity, which have been studied by electrical resistivity and ac calorimetry under nearly hydrostatic environments. Compared with its polycrystalline counterpart, bulk superconductivity coexists with antiferromagnetism in a much narrower pressure region. The possible existence of textured superconductivity and local quantum criticality also are observed in CePt2In7, exhibiting a remarkable similarity with CeRhIn5.

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arXiv2012

PuPt2In7: a computational and experimental investigation

Flux-grown single crystals of PuPt$_2$In$_7$ are characterized and found to be both non-superconducting and non-magnetic down to 2 K. The Sommerfeld specific heat coefficient of $\sim 250$ mJ/mol K$^2$ indicates heavy fermion behavior. We report the results of generalized gradient approximation (GGA)+$U$ calculations of PuPt$_2$In$_7$ and as yet unsynthesized isovalent PuPt$_2$Ga$_7$. The strength of the $c$-$f$ hybridization of PuPt$_2$In$_7$ is similar to the PuCoIn$_5$ superconductor. The bare and $f$-weighted susceptibility within the constant-matrix-element approximation is calculated, showing a maximum along the $q_z$ direction at $q_x = q_y = 0.5$. A similar and slightly stronger maximum is also found in the structurally related heavy-fermion materials PuCoGa$_5$ and PuCoIn$_5$. The absence of superconductivity in PuPt$_2$In$_7$ is examined based on the results of our calculations.

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arXiv2012

Electronic tuning and uniform superconductivity in CeCoIn5

We report a globally reversible effect of electronic tuning on the magnetic phase diagram in CeCoIn_{5} driven by electron (Pt and Sn) and hole (Cd, Hg) doping. Consequently, we are able to extract the superconducting pair breaking component for hole and electron dopants with pressure and co-doping studies, respectively. We find that these nominally non-magnetic dopants have a remarkably weak pair breaking effect for a d-wave superconductor. The pair breaking is weaker for hole dopants, which induce magnetic moments, than for electron dopants. Furthermore, both Pt and Sn doping have a similar effect on superconductivity despite being on different dopant sites, arguing against the notion that superconductivity lives predominantly in the CeIn_{3} planes of these materials. In addition, we shed qualitative understanding on the doping dependence with density functional theory calculations.

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arXiv2012

Controllable chirality-induced geometrical Hall effect in a frustrated highly-correlated metal

A current of electrons traversing a landscape of localized spins possessing non-coplanar magnetic order gains a geometrical (Berry) phase which can lead to a Hall voltage independent of the spin-orbit coupling within the material--a geometrical Hall effect. We show that the highly-correlated metal UCu5 possesses an unusually large controllable geometrical Hall effect at T<1.2K due to its frustration-induced magnetic order. The magnitude of the Hall response exceeds 20% of the ν=1 quantum Hall effect per atomic layer, which translates into an effective magnetic field of several hundred Tesla acting on the electrons. The existence of such a large geometric Hall response in UCu5 opens a new field of inquiry into the importance of the role of frustration in highly-correlated electron materials.

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arXiv2012

Multiconfigurational nature of 5f orbitals in uranium and plutonium intermetallics

Uranium and plutonium's 5f electrons are tenuously poised between strongly bonding with ligand spd-states and residing close to the nucleus. The unusual properties of these elements and their compounds (eg. the six different allotropes of elemental plutonium) are widely believed to depend on the related attributes of f-orbital occupancy and delocalization, for which a quantitative measure is lacking. By employing resonant x-ray emission spectroscopy (RXES) and x-ray absorption near-edge structure (XANES) spectroscopy and making comparisons to specific heat measurements, we demonstrate the presence of multiconfigurational f-orbital states in the actinide elements U and Pu, and in a wide range of uranium and plutonium intermetallic compounds. These results provide a robust experimental basis for a new framework for understanding the strongly-correlated behavior of actinide materials.

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