arXiv subjects

W. A. Phelan

Publications and source records attributed to W. A. Phelan.

13 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.

cond-mat.str-el↗

arXiv2023

Topological surface states in the Kondo insulator YbB$_{12}$ revealed via planar tunneling spectroscopy

Planar tunneling spectroscopy of the Kondo insulator SmB$_6$ suggests that an interaction between the surface Dirac fermions and the bulk spin excitons results in incompletely protected topological surface states. To gain further insight into their true nature, it is necessary to study other topological Kondo insulator candidates. Calculations of electronic energy bands predict that the Kondo insulator YbB$_{12}$ hosts topological surface states protected by crystalline mirror symmetry. In this study, we present tunneling conductance spectra obtained from the (001) surface of YbB$_{12}$ single crystals and discuss them in comparison to SmB$_6$. The linear conductance at low bias provides strong evidence for the existence of surface Dirac fermions. The double-hump structure in the negative bias region is associated with hybridized band edges, in agreement with a calculated band structure. While these similarities with SmB6 are suggestive of the existence of topological surface states in YbB$_{12}$, in agreement with other experiments, some discrepancies are also observed, which we attribute to a difference in their exact nature from those in SmB$_6$.

cond-mat.str-el↗

arXiv2021

Topological nature of the Kondo insulator SmB$_6$ and its sensitiveness to Sm vacancy

The true topological nature of the Kondo insulator SmB$_6$ remains to be unveiled. Our previous tunneling study not only found evidence for the existence of surface Dirac fermions, but it also uncovered that they inherently interact with the spin excitons, collective excitations in the bulk. We have extended such a spectroscopic investigation into crystals containing a Sm deficiency. The bulk hybridization gap is found to be insensitive to the deficiency up to 1% studied here, but the surface states in Sm-deficient crystals exhibit quite different temperature evolutions from those in stoichiometric ones. We attribute this to the topological surface states remaining incoherent down to the lowest measurement temperature due to their continued interaction with the spin excitons that remain uncondensed. This result shows that the detailed topological nature of SmB$_6$ could vary drastically in the presence of disorder in the lattice. This sensitiveness to disorder is seemingly contradictory to the celebrated topological protection, but it can be understood as being due to the intimate interplay between strong correlations and topological effects.

cond-mat.str-el↗

arXiv2020

Helical magnetic order and Fermi surface nesting in non-centrosymmetric ScFeGe

An investigation of the structural, magnetic, thermodynamic, and charge transport properties of non-centrosymmetric hexagonal ScFeGe reveals it to be an anisotropic metal with a transition to a weak itinerant incommensurate helimagnetic state below $T_N = 36$ K. Neutron diffraction measurements discovered a temperature and field independent helical wavevector \textbf{\textit{k}} = (0 0 0.193) with magnetic moments of 0.53 $μ_{B}$ per formula unit confined to the {\it ab}-plane. Density functional theory calculations are consistent with these measurements and find several bands that cross the Fermi level along the {\it c}-axis with a nearly degenerate set of flat bands just above the Fermi energy. The anisotropy found in the electrical transport is reflected in the calculated Fermi surface, which consists of several warped flat sheets along the $c$-axis with two regions of significant nesting, one of which has a wavevector that closely matches that found in the neutron diffraction. The electronic structure calculations, along with a strong anomaly in the {\it c}-axis conductivity at $T_N$, signal a Fermi surface driven magnetic transition, similar to that found in spin density wave materials. Magnetic fields applied in the {\it ab}-plane result in a metamagnetic transition with a threshold field of $\approx$ 6.7 T along with a sharp, strongly temperature dependent, discontinuity and a change in sign of the magnetoresistance for in-plane currents. Thus, ScFeGe is an ideal system to investigate the effect of in-plane magnetic fields on an easy-plane magnetic system, where the relative strength of the magnetic interactions and anisotropies determine the topology and magnetic structure.

cond-mat.mtrl-sci↗

arXiv2019

Incommensurate magnetism near quantum criticality in CeNiAsO

Two phase transitions in the tetragonal strongly correlated electron system CeNiAsO were probed by neutron scattering and zero field muon spin rotation. For $T <T_{N1}$ = 8.7(3) K, a second order phase transition yields an incommensurate spin density wave with wave vector $\textbf{k} = (0.44(4), 0, 0)$. For $T < T_{N2}$ = 7.6(3) K, we find co-planar commensurate order with a moment of $0.37(5)~μ_B$, reduced to $30 \%$ of the saturation moment of the $|\pm\frac{1}{2}\rangle$ Kramers doublet ground state, which we establish by inelastic neutron scattering. Muon spin rotation in $\rm CeNiAs_{1-x}P_xO$ shows the commensurate order only exists for x $\le$ 0.1 so the transition at $x_c$ = 0.4(1) is from an incommensurate longitudinal spin density wave to a paramagnetic Fermi liquid.

cond-mat.str-el↗

arXiv2018

Field-dependent heat transport in the Kondo insulator SmB6 : phonons scattered by magnetic impurities

The thermal conductivity $κ$ of the Kondo insulator SmB$_6$ was measured at low temperature, down to 70 mK, in magnetic fields up to 15 T, on single crystals grown using both the floating-zone and the flux methods. The residual linear term $κ_0/T$ at $T \to 0$ is found to be zero in all samples, for all magnetic fields, in agreement with previous studies. There is therefore no clear evidence of fermionic heat carriers. In contrast to some prior data, we observe a large enhancement of $κ(T)$ with increasing field. The effect of field is anisotropic, depending on the relative orientation of field and heat current (parallel or perpendicular), and with respect to the cubic crystal structure. We interpret our data in terms of heat transport predominantly by phonons, which are scattered by magnetic impurities.

cond-mat.str-el↗

arXiv2017

Impurities or a neutral Fermi surface? A further examination of the low-energy ac optical conductivity of SmB$_6$

Recent experiments have uncovered evidence of low energy excitations in the bulk of SmB$_6$ that are perhaps associated with unconventional quasiparticles, bringing into question whether this Kondo "insulator" is truly insulating in the bulk. Recently, we demonstrated that SmB$_6$ possesses significant in-gap bulk ac conduction far in excess of typical disordered semiconductors. Whether such conduction is an intrinsic feature of SmB$_6$, suggesting the formation of an exotic state, or residual conduction from impurities continues to be a topic of debate. Here, we further examine the origin of the ac optical conductivity of SmB$_6$ in light of recent experimental and theoretical developments. The optical conductivity of SmB$_6$ is shown to possess distinct regimes of either dominant free carrier or $localized$ response contributions. The free carrier response is found to be in good qualitative agreement with previous literature, although quantitative differences are revealed and discussed. The localized response, which dominates at the lowest temperatures, is analyzed in the context of models of either in-gap impurity states or an exotic neutral Fermi surface. The charge density or effective mass of this low temperature in-gap conductivity is extracted through a conductivity sum rule analysis and found to be in general alignment with both models in the appropriate limits. Our results shed further light on the nature of the in-gap states of this remarkable material.

cond-mat.str-el↗

arXiv2017

A magnetic topological semimetal Sr1-yMn1-zSb2 (y, z< 0.1)

Weyl (WSMs) evolve from Dirac semimetals in the presence of broken time-reversal symmetry (TRS) or space-inversion symmetry. The WSM phases in TaAs-class materials and photonic crystals are due to the loss of space-inversion symmetry. For TRS-breaking WSMs, despite numerous theoretical and experimental efforts, few examples have been reported. In this Article, we report a new type of magnetic semimetal Sr1-yMn1-zSb2 (y,z<0.1) with nearly massless relativistic fermion behaviour (m*=0.04-0.05m0, where m0 is the free electron mass). This material exhibits a ferromagnetic order for 304K < T < 565K, but a canted antiferromagnetic order with a ferromagnetic component for T < 304K. The combination of relativistic fermion behaviour and ferromagnetism in Sr1-yMn1-zSb2 offers a rare opportunity to investigate the interplay between relativistic fermions and spontaneous TRS breaking.

cond-mat.mtrl-sci↗

arXiv2017

Effect of Negative Pressure on the Prototypical Itinerant Magnet MnSi

The evolution of the magnetic and charge transport properties of itinerant magnetic metal MnSi with the substitution of Al and Ga on the Si site is investigated. We observe an increase in unit cell volume indicating that both Al and Ga substitutions create negative chemical pressure. There are substantial increases in the Curie temperature and the ordered moment demonstrating that the substitutions give the magnetism a more local character. The substitutions also increase the range of temperature and field where the skyrmion phase is stable due to a change in the character of the magnetism. In contrast to the behavior of pure MnSi and expectations for the intrinsic anomalous Hall effect, we find a significant temperature dependence to the magnitude and sign of anomalous Hall conductivity constant in Al or Ga substituted samples. This temperature dependence likely reflects changes in the spin-orbit coupling strength with temperature, which may have significant consequences on the helical and skyrmion states. Overall, we observe a continuous evolution of magnetic and charge transport properties through positive to negative pressure

cond-mat.mtrl-sci↗

arXiv2016

Anomalous 3D bulk AC conduction within the Kondo gap of SmB$_6$ single crystals

The Kondo insulator SmB$_6$ has long been known to display anomalous transport behavior at low temperatures, T$<5$ K. In this temperatures range, a plateau is observed in the dc resistivity, contrary to the exponential divergence expected for a gapped system. Recent theoretical calculations suggest that SmB$_6$ may be the first topological Kondo insulator (TKI) and propose that the residual conductivity is due to topological surface states which reside within the Kondo gap. Since the TKI prediction many experiments have claimed to observe high mobility surface states within a perfectly insulating hybridization gap. Here, we investigate the low energy optical conductivity within the hybridization gap of single crystals of SmB$_6$ via time domain terahertz spectroscopy. Samples grown by both optical floating zone and aluminum flux methods are investigated to probe for differences originating from sample growth techniques. We find that both samples display significant 3D bulk conduction originating within the Kondo gap. Although SmB$_6$ may be a bulk dc insulator, it shows significant bulk ac conduction that is many orders of magnitude larger than any known impurity band conduction. The nature of these in-gap states and their coupling with the low energy spin excitons of SmB$_6$ is discussed. Additionally, the well defined conduction path geometry of our optical experiments allows us to show that any surface states, which lie below our detection threshold if present, must have a sheet resistance of R$/\square \ge$ 1000 $Ω$.

cond-mat.str-el↗

arXiv2015

On the Chemistry and Physical Properties of Flux and Floating Zone Grown SmB6 Single Crystals

Recent theoretical and experimental findings suggest that the long-known but not well understood low temperature resistance plateau of SmB6 may originate from protected surface states arising from a topologically non-trivial bulk band structure having strong Kondo hybridization. Yet other studies have ascribed this feature to impurity phases, sample vacancies, and surface reconstructions. Given the typical methods used to prepare SmB6 single crystals, the flux and floating zone procedures, these ascriptions should not be taken lightly. Here, we demonstrate how compositional variations and observable amounts of impurity phases in SmB6 crystals grown by floating zone and flux affect the physical properties. From neutron diffraction and X-ray computed tomography experiments, we observe that a 154Sm11B6 crystal prepared using aluminum flux contains co-crystallized, epitaxial aluminum. A large, nearly stoichiometric crystal of SmB6 was successfully grown using the float-zone technique; upon continuing the zone melting, samarium vacancies are introduced. These samarium vacancies drastically alter the resistance and plateauing magnitude of the low temperature resistance compared to stoichiometric SmB6. These results highlight that small presences of impurity phases and compositional variations must be considered when collecting and analyzing physical property data of SmB6. Finally, a more accurate samarium-154 coherent neutron scattering length value, 8.9(1) fm, is reported.

cond-mat.str-el↗

arXiv2014

Correlation between bulk thermodynamic measurements and the low temperature resistance plateau in SmB6

Topological insulators are materials characterized by dissipationless, spin-polarized surface states resulting from non-trivial band topologies. Recent theoretical models and experiments suggest that SmB6 is the first topological Kondo insulator, in which the topologically non-trivial band structure results from electron-electron interactions via Kondo hybridization. Here, we report that the surface conductivity of SmB6 increases systematically with bulk carbon content. Further, addition of carbon is linked to an increase in n-type carriers, larger low temperature electronic contributions to the specific heat with a characteristic temperature scale of T* = 17 K, and a broadening of the crossover to the insulating state. Additionally, X-ray absorption spectroscopy shows a change in Sm valence at the surface. Our results highlight the importance of phonon dynamics in producing a Kondo insulating state and demonstrate a correlation between the bulk thermodynamic state and low temperature resistance of SmB6.

cond-mat.str-el↗

arXiv2013

Thermoelectric Properties of Intermetallic Semiconducting RuIn3 and Metallic IrIn3

Low temperature (<400 K) thermoelectric properties of semiconducting RuIn3 and metallic IrIn3 are reported. RuIn3 is a narrow band gap semiconductor with a large n-type Seebeck coefficient at room temperature (S(290K)~400 μV/K), but the thermoelectric Figure of merit (ZT(290K) = 0.007) is small because of high electrical resistivity and thermal conductivity (κ(290 K) ~ 2.0 W/m K). IrIn3 is a metal with low thermopower at room temperature (S(290K)~20 μV/K) . Iridium substitution on the ruthenium site has a dramatic effect on transport properties, which leads to a large improvement in the power factor and corresponding Figure of merit (ZT(380 K) = 0.053), improving the efficiency of the material by an over of magnitude.

cond-mat.mtrl-sci↗