Mn substitution in the topological metal Zr2Te2P.

Results are reported for Mn intercalated Zr2Te2P, where x-ray diffraction , energy dispersive spectroscopy, and transmission electron microscopy measurements reveal that the van der Waals bonded Te-Te layers are partially filled by Zr and Mn ions. This leads to the chemical formulas Zr0.07Zr2Te2P and Mn0.06Zr0.03Zr2Te2P for the parent and substituted compounds, respectively. The impact of the Mn ions is seen in the anisotropic magnetic susceptibility, where Curie-Weiss fits to the data indicate that the Mn ions are in the divalent state. Heat capacity and electrical transport measurements reveal metallic behavior, but the electronic coefficient of the heat capacity (γMn≈ 36.6 mJ (mol·K2)-1) is enhanced by comparison to that of the parent compound. Magnetic ordering is seen atTM≈4 K, where heat capacity measurements additionally show that the phase transition is broad, likely due to the disordered Mn distribution. This transition also strongly reduces the electronic scattering seen in the normalized electrical resistance. These results show that Mn substitution simultaneously introduces magnetic interactions and tunes the electronic state, which improves prospects for inducing novel behavior in Zr2Te2P and the broader family of ternary tetradymites.

Resonance from antiferromagnetic spin fluctuations for superconductivity in UTe2.

Superconductivity originates from the formation of bound (Cooper) pairs of electrons that can move through the lattice without resistance below the superconducting transition temperature Tc (ref. 1). Electron Cooper pairs in most superconductors form anti-parallel spin singlets with total spin S = 0 (ref. 2), although they can also form parallel spin-triplet Cooper pairs with S = 1 and an odd parity wavefunction3. Spin-triplet pairing is important because it can host topological states and Majorana fermions relevant for quantum computation4,5. Because spin-triplet pairing is usually mediated by ferromagnetic (FM) spin fluctuations3, uranium-based materials near an FM instability are considered to be ideal candidates for realizing spin-triplet superconductivity6. Indeed, UTe2, which has a Tc ≈ 1.6 K (refs. 7,8), has been identified as a candidate for a chiral spin-triplet topological superconductor near an FM instability7-14, although it also has antiferromagnetic (AF) spin fluctuations15,16. Here we use inelastic neutron scattering (INS) to show that superconductivity in UTe2 is coupled to a sharp magnetic excitation, termed resonance17-23, at the Brillouin zone boundary near AF order. Because the resonance has only been found in spin-singlet unconventional superconductors near an AF instability17-23, its observation in UTe2 suggests that AF spin fluctuations may also induce spin-triplet pairing24 or that electron pairing in UTe2 has a spin-singlet component.

Experimental Observation and Spin Texture of Dirac Node Arcs in Tetradymite Topological Metals.

We report the observation of a nontrivial spin texture in Dirac node arcs, i.e., novel topological objects formed when Dirac cones of massless particles extend along an open one-dimensional line in momentum space. We find that such states are present in all the compounds of the tetradymite M_{2}Te_{2}X family (M=Ti, Zr, or Hf and X=P or As) regardless of the weak or strong character of the topological invariant. The Dirac node arcs in tetradymites are thus the simplest possible textbook example of a type-I Dirac system with a single spin-polarized node arc.

Electronic and magnetic properties of EuNi2-δ Sb2 structural variants.

X-ray diffraction, magnetic susceptibility, magnetization, heat capacity and electrical resistivity results are reported for single crystals of two structural variants of EuNi2-δ Sb2 that crystallize in the CaBe2Ge2 and ThCr2Si2-type structures. While the former occurs with a stoichiometric ratio, the latter exhibits a Ni site vacancy (δ = 0.36). Both systems exhibit similar magnetic behavior at elevated temperatures, where there is an isotropic Curie-Weiss temperature dependence that indicates an antiferromagnetic exchange interaction between divalent europium ions, although it is stronger for the CaBe2Ge2-variant. At low temperatures, the differing structural environments that surround the Eu ions result in distinct ordering behavior. The CaBe2Ge2-variant orders antiferromagnetically near T N1 = 6.9 K and then undergoes a first order phase transition at T M = 4.6 K. The ThCr2Si2-variant exhibits simpler behavior, with antiferromagnetic ordering at T N2 = 5.6 K. For both compounds, an applied magnetic field suppresses the ordering temperatures and induce metamagnetic phase transitions, while applied pressure causes the ordering temperatures to increase. From these results, EuNi2-δ Sb2 emerges as a useful system in which to study the impact of structural variation on magnetism in a Eu-based metal.

Superconductivity in a uranium containing high entropy alloy.

High entropy alloys (HEA) are an unusual class of materials where mixtures of elements are stochastically arrayed on a simple crystalline lattice. These systems exhibit remarkable functionality, often along several distinct axes: e.g., the examples [TaNb]1-x(TiZrHf)x are high strength and damage resistant refractory metals that also exhibit superconductivity with large upper critical fields. Here we report the discovery of an f-electron containing HEA, [TaNb]0.31(TiUHf)0.69, which is the first to include an actinide ion. Similar to the Zr-analogue, this material crystallizes in a body-centered cubic lattice with the lattice constant a = 3.41(1) Å and exhibits phonon mediated superconductivity with a transition temperatures Tc ≈ 3.2 K and upper critical fields Hc2 ≈ 6.4 T. These results expand this class of materials to include actinide elements, shows that superconductivity is robust in this sub-group, and opens the path towards leveraging HEAs as functional waste forms for a variety of radioisotopes.

A novel cage for actinides: A 6W4Al43 (A = U and Pu).

We report on synthesis and characterization of the compounds A 6W4Al43 (A = U and Pu), that form in the hexagonal Ho6Mo4Al43 caged-structure family. The A ions reside within W/Al cages where the A-A nearest neighbors form dimers between adjacent W/Al cages, with U-U and Pu-Pu distances of 3.3892 [Formula: see text] and 3.4080 [Formula: see text], respectively. While the W/Al networks provide environments similar to those of other cage-like materials (e.g. filled skutterudites), the atomic displacement parameters from single crystal x-ray diffraction measurements show that the A-ions do not exhibit rattling behavior. We find that there is site interchange disorder on one of the W/Al sites. Magnetic susceptibility measurements show that U6W4Al43 displays anisotropic Curie-Weiss behavior where it fits to the data yield an effective magnetic moment near 2.0 [Formula: see text]/U. At low temperatures the magnetic susceptibility deviates from the Curie-Weiss temperature dependence and eventually saturates to a constant value. In contrast, Pu6W4Al43 displays nearly temperature independent Pauli paramagnetism for all temperatures, as would be expected if the 5f -electrons are delocalized. The electrical resistivity for U6W4Al43 increases slightly with the decreasing temperature, suggesting that it is dominated by f -electronic hybridization effects and disorder scattering that originates from the W/Al site interchange. Specific heat measurements for U6W4Al43 further reveal an enhanced electronic Sommerfeld coefficient that is consistent with a moderately enhanced charge carrier effective mass. Together these measurements expose these materials as hosts for unstable f -electron magnetism, where the novel cage-like structures control the phenomena through the spacing between the A ions. Through this combination of mild magnetism, the low cost elements of the Al-W cages, and chemical tunability that has been shown for related materials in the same structure, the A 6W4Al43 compounds emerge as promising nuclear waste-forms for transuranics, while the wider family of materials makes an appealing environment for studying f -electron physics in a novel structure.

Bulk Fermi Surfaces of the Dirac Type-II Semimetallic Candidates MAl_{3} (Where M=V, Nb, and Ta).

We report a de Haas-van Alphen (dHvA) effect study on the Dirac type-II semimetallic candidates MAl_{3} (where, M=V, Nb and Ta). The angular dependence of their Fermi surface (FS) cross-sectional areas reveals a remarkably good agreement with our first-principles calculations. Therefore, dHvA supports the existence of tilted Dirac cones with Dirac type-II nodes located at 100, 230 and 250 meV above the Fermi level ϵ_{F} for VAl_{3}, NbAl_{3} and TaAl_{3} respectively, in agreement with the prediction of broken Lorentz invariance in these compounds. However, for all three compounds we find that the cyclotron orbits on their FSs, including an orbit nearly enclosing the Dirac type-II node, yield trivial Berry phases. We explain this via an analysis of the Berry phase where the position of this orbit, relative to the Dirac node, is adjusted within the error implied by the small disagreement between our calculations and the experiments. We suggest that a very small amount of doping could displace ϵ_{F} to produce topologically nontrivial orbits encircling their Dirac node(s).

Domain engineering of the metastable domains in the 4f-uniaxial-ferromagnet CeRu2Ga2B.

In search of novel, improved materials for magnetic data storage and spintronic devices, compounds that allow a tailoring of magnetic domain shapes and sizes are essential. Good candidates are materials with intrinsic anisotropies or competing interactions, as they are prone to host various domain phases that can be easily and precisely selected by external tuning parameters such as temperature and magnetic field. Here, we utilize vector magnetic fields to visualize directly the magnetic anisotropy in the uniaxial ferromagnet CeRu2Ga2B. We demonstrate a feasible control both globally and locally of domain shapes and sizes by the external field as well as a smooth transition from single stripe to bubble domains, which opens the door to future applications based on magnetic domain tailoring.

Thermodynamic and electrical transport investigation of URu2Si2-x P x.

Magnetic susceptibility, electrical resistivity, and heat capacity results are reported for the chemical substitution series URu2Si2-x P x for [Formula: see text]. This study expands in detail on work recently reported in Gallagher et al (2016 Nat. Commun. 10712), which focused on the small x region of this substitution series. Measurements presented here reveal persistent hybridization between the f- and conduction electrons and strong variation of the low temperature behavior with increasing x. Hidden order and superconductivity are rapidly destroyed for [Formula: see text] and are replaced for [Formula: see text] by a region with Kondo coherence but no ordered state. Antiferromagnetism abruptly appears for [Formula: see text]. This phase diagram differs significantly from those produced by most other tuning strategies in URu2Si2, including applied pressure, high magnetic fields, and isoelectronic chemical substitution (i.e. Ru → Fe and Os), where hidden order and magnetism share a common phase boundary. Besides revealing an intriguing evolution of the low temperature states, this series provides a setting in which to investigate the influence of electronic tuning, where probes that are sensitive to the Fermi surface and the symmetry of the ordered states will be useful to unravel the anomalous behavior of URu2Si2.

Candidate Elastic Quantum Critical Point in LaCu_{6-x}Au_{x}.

The structural properties of LaCu_{6-x}Au_{x} are studied using neutron diffraction, x-ray diffraction, and heat capacity measurements. The continuous orthorhombic-monoclinic structural phase transition in LaCu_{6} is suppressed linearly with Au substitution until a complete suppression of the structural phase transition occurs at the critical composition x_{c}=0.3. Heat capacity measurements at low temperatures indicate residual structural instability at x_{c}. The instability is ferroelastic in nature, with density functional theory calculations showing negligible coupling to electronic states near the Fermi level. The data and calculations presented here are consistent with the zero temperature termination of a continuous structural phase transition suggesting that the LaCu_{6-x}Au_{x} series hosts an elastic quantum critical point.

Quantum Critical Scaling in the Disordered Itinerant Ferromagnet UCo_{1-x}Fe_{x}Ge.

The Belitz-Kirkpatrick-Vojta (BKV) theory shows in excellent agreement with experiment that ferromagnetic quantum phase transitions (QPTs) in clean metals are generally first order due to the coupling of the magnetization to electronic soft modes, in contrast to the classical analogue that is an archetypical second-order phase transition. For disordered metals the BKV theory predicts that the second-order nature of the QPT is restored because the electronic soft modes change their nature from ballistic to diffusive. Our low-temperature magnetization study identifies the ferromagnetic QPT in the disordered metal UCo_{1-x}Fe_{x}Ge as the first clear example that exhibits the associated critical exponents predicted by the BKV theory.

Electrical and thermal transport properties of the electron-doped cuprate Sm2-x Ce x CuO4-y system.

Electrical and thermal transport measurements were performed on thin films of the electron-doped superconductor Sm2-x Ce x CuO4-y (x = 0.13 - 0.19) in order to study the evolving nature of the charge carriers from the under-doped to over-doped regime. A temperature versus cerium content (T - x) phase diagram has been constructed from the electrical transport measurements, yielding a superconducting region similar to that found for other electron-doped superconductors. Thermopower measurements show a dramatic change from the underdoped region (x < 0.15) to the overdoped region (x > 0.15). Application of the Fisher-Fisher-Huse (FFH) vortex glass scaling model to the magnetoresistance data was found to be insufficient to describe the data in the region of the vortex-solid to vortex-liquid transition. It was found instead that the modified vortex glass scaling model of Rydh, Rapp, and Anderson provided a good description of the data, indicating the importance of the applied field on the pinning landscape. A magnetic field versus temperature (H - T) phase diagram has also been constructed for the films with [Formula: see text], displaying the evolution of the vortex glass melting lines H g (T) across the superconducting regime.

Interplanar coupling-dependent magnetoresistivity in high-purity layered metals.

The magnetic field-induced changes in the conductivity of metals are the subject of intense interest, both for revealing new phenomena and as a valuable tool for determining their Fermi surface. Here we report a hitherto unobserved magnetoresistive effect in ultra-clean layered metals, namely a negative longitudinal magnetoresistance that is capable of overcoming their very pronounced orbital one. This effect is correlated with the interlayer coupling disappearing for fields applied along the so-called Yamaji angles where the interlayer coupling vanishes. Therefore, it is intrinsically associated with the Fermi points in the field-induced quasi-one-dimensional electronic dispersion, implying that it results from the axial anomaly among these Fermi points. In its original formulation, the anomaly is predicted to violate separate number conservation laws for left- and right-handed chiral (for example, Weyl) fermions. Its observation in PdCoO2, PtCoO2 and Sr2RuO4 suggests that the anomaly affects the transport of clean conductors, in particular near the quantum limit.

Uncovering the behavior of Hf2Te2P and the candidate Dirac metal Zr2Te2P.

Results are reported for single crystal specimens of Hf2Te2P and compared to its structural analogue Zr2Te2P, which was recently proposed to be a potential reservoir for Dirac physics [1]. Both materials are produced using the iodine vapor phase transport method and the resulting crystals are exfoliable. The bulk electrical transport and thermodynamic properties indicate Fermi liquid behavior at low temperature for both compounds. Quantum oscillations are observed in magnetization measurements for fields applied parallel but not perpendicular to the c-axis, suggesting that the Fermi surfaces are quasi-two dimensional. Frequencies are determined from quantum oscillations for several parts of the Fermi surfaces. Lifshitz-Kosevich fits to the temperature dependent amplitudes of the oscillations reveal small effective masses, with a particularly small value [Formula: see text] for the α branch of Zr2Te2P. Electronic structure calculations are in good agreement with quantum oscillation results and illustrate the effect of a stronger spin-orbit interaction going from Zr to Hf. These results suggest that by using appropriate tuning parameters this class of materials may deepen the pool of novel Dirac phenomena.

Unfolding the physics of URu2Si2 through silicon to phosphorus substitution.

The heavy fermion intermetallic compound URu2Si2 exhibits a hidden-order phase below the temperature of 17.5 K, which supports both anomalous metallic behavior and unconventional superconductivity. While these individual phenomena have been investigated in detail, it remains unclear how they are related to each other and to what extent uranium f-electron valence fluctuations influence each one. Here we use ligand site substituted URu2Si(2-x)P(x) to establish their evolution under electronic tuning. We find that while hidden order is monotonically suppressed and destroyed for x≤0.035, the superconducting strength evolves non-monotonically with a maximum near x≈0.01 and that superconductivity is destroyed near x≈0.028. This behavior reveals that hidden order depends strongly on tuning outside of the U f-electron shells. It also suggests that while hidden order provides an environment for superconductivity and anomalous metallic behavior, it's fluctuations may not be solely responsible for their progression.

Frustrated magnetism in the spin-chain metal Yb2Fe12P7.

Magnetization measurements for magnetic fields [Formula: see text] up to 60 T are reported for the noncentrosymmetric spin-chain metal Yb2Fe12P7. These measurements reveal behavior that is consistent with Ising-like spin chain magnetism that produces pronounced spin degeneracy. In particular, we find that although a Brillouin field dependence is observed in M(H) for [Formula: see text] with a saturation moment that is close to the expected value for free ions of Yb(3+) , non-Brillouin-like behavior is seen for [Formula: see text] with an initial saturation moment that is nearly half the free ion value. In addition, hysteretic behavior that extends above the ordering temperature [Formula: see text] is seen for [Formula: see text] but not for [Formula: see text], suggesting out-of-equilibrium physics. This point of view is strengthened by the observation of a spin reconfiguration in the ordered state for [Formula: see text] which is only seen for [Formula: see text] and after polarizing the spins. Together with the heat capacity data, these results suggest that the anomalous low temperature phenomena that were previously reported (Baumbach 2010 et al Phys. Rev. Lett. 105 106403) are driven by spin degeneracy that is related to the Ising-like one dimensional chain-like configuration of the Yb ions.

Evidence for a nematic component to the hidden-order parameter in URu2Si2 from differential elastoresistance measurements.

For materials that harbour a continuous phase transition, the susceptibility of the material to various fields can be used to understand the nature of the fluctuating order and hence the nature of the ordered state. Here we use anisotropic biaxial strain to probe the nematic susceptibility of URu2Si2, a heavy fermion material for which the nature of the low temperature 'hidden order' state has defied comprehensive understanding for over 30 years. Our measurements reveal that the fluctuating order has a nematic component, confirming reports of twofold anisotropy in the broken symmetry state and strongly constraining theoretical models of the hidden-order phase.

Heavy fermions. Chirality density wave of the "hidden order" phase in URu2Si2.

A second-order phase transition in a physical system is associated with the emergence of an "order parameter" and a spontaneous symmetry breaking. The heavy fermion superconductor URu2Si2 has a "hidden order" (HO) phase below the temperature of 17.5 kelvin; the symmetry of the associated order parameter has remained ambiguous. Here we use polarization-resolved Raman spectroscopy to specify the symmetry of the low-energy excitations above and below the HO transition. We determine that the HO parameter breaks local vertical and diagonal reflection symmetries at the uranium sites, resulting in crystal field states with distinct chiral properties, which order to a commensurate chirality density wave ground state.

Quantum critical fluctuations in the heavy fermion compound Ce(Ni0.935Pd0.065)2Ge2.

Electric resistivity, specific heat, magnetic susceptibility, and inelastic neutron scattering experiments were performed on a single crystal of the heavy fermion compound Ce(Ni0.935Pd0.065)2Ge2 in order to study the spin fluctuations near an antiferromagnetic (AF) quantum critical point (QCP). The resistivity and the specific heat coefficient for T ⩽ 1 K exhibit the power law behavior expected for a 3D itinerant AF QCP (ρ(T) ∼ T(3/2) and γ(T) ∼ γ0 - bT(1/2)). However, for 2 ⩽ T ⩽ 10 K, the susceptibility and specific heat vary as log T and the resistivity varies linearly with temperature. Furthermore, despite the fact that the resistivity and specific heat exhibit the non-Fermi liquid behavior expected at a QCP, the correlation length, correlation time, and staggered susceptibility of the spin fluctuations remain finite at low temperature. We suggest that these deviations from the divergent behavior expected for a QCP may result from alloy disorder.

Single crystal study of antiferromagnetic CePd3Al9.

Single crystal x-ray diffraction, magnetic susceptibility (M), heat capacity (C), and electrical resistivity (ρ) measurements are reported for specimens of the new tetragonal compound CePd3Al9, which forms in a new structure type. X-ray diffraction measurements reveal that the nearest neighbor Ce-Ce distances are large (d(Ce-Ce) = 5.272 Å), suggesting that this compound may be described as a stoichiometric dilute Kondo lattice. Thermodynamic and transport measurements reveal antiferromagnetic order near T(N) = 0.9 K. The ordered ground state emerges from a lattice of localized Ce ions that are weakly hybridized with the conduction electrons, as revealed by the moderate electronic coefficient of the specific heat γ ≈ 45 mJ mol(-1) K(-2) (extrapolated from above T(N)) and the lack of evidence for Kondo coherence in the magnetic susceptibility and electrical resistivity. The application of a magnetic field initially suppresses the magnetic order at a rate of -0.04 K kOe(-1), but Zeeman splitting of the doublet ground state produces a nonmagnetic singlet before TN reaches zero. The data additionally reveal that chemical/structural disorder plays an important role, as evidenced by results from single crystal x-ray diffraction, the broadness of the peak at TN in the heat capacity, and the small residual resistivity ratio RRR = ρ(300 K)/ρ0 = 1.3.