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Homogeneous mixed-valence (MV) behaviour is one of the most intriguing phenomena of f-electron systems. Despite extensive efforts, a fundamental aspect which remains unsettled is the experimental determination of the limiting cases for which MV emerges. Here we address this question for SmB6, a prototypical MV system characterized by two nearly-degenerate Sm2+ and Sm3+ configurations. By combining angle-resolved photoemission spectroscopy (ARPES) and x-ray absorption spectroscopy (XAS), we track the evolution of the mean Sm valence, vSm, in the SmxLa1-xB6 series. Upon substitution of Sm ions with trivalent La, we observe a linear decrease of valence fluctuations to an almost complete suppression at x = 0.2, with vSm ~ 2; surprisingly, by further reducing x, a re-entrant increase of vSm develops, approaching the value of vimp ~ 2.35 in the dilute-impurity limit. Such behaviour departs from a monotonic evolution of vSm across the whole series, as well as from the expectation of its convergence to an integer value for x â 0. Our ARPES and XAS results, complemented by a phenomenological model, demonstrate an unconventional evolution of the MV character in the SmxLa1-xB6 series, paving the way to further theoretical and experimental considerations on the concept of MV itself, and its influence on the macroscopic properties of rare-earth compounds in the dilute-to-intermediate impurity regime.
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We have investigated the low-temperature local magnetic properties in the bulk of molten salt-flux (MSF)-grown single crystals of the candidate odd-parity superconductor UTe_{2} by zero-field muon spin relaxation (µSR). In contrast to previous µSR studies of UTe_{2} single crystals grown by a chemical vapor transport method, we find no evidence of magnetic clusters or electronic moments fluctuating slow enough to cause a discernible relaxation of the zero-field µSR asymmetry spectrum. Consequently, our measurements on MSF-grown single crystals rule out the generation of spontaneous magnetic fields in the bulk that would occur near impurities or lattice defects if the superconducting state of UTe_{2} breaks time-reversal symmetry. This result suggests that UTe_{2} is characterized by a single-component superconducting order parameter.
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We study the interplay between electronic correlations and hybridization in the low-energy electronic structure of CaMn[Formula: see text]Bi[Formula: see text], a candidate hybridization-gap semiconductor. By employing a DFT+U approach we find both the antiferromagnetic Néel order and band gap in good agreement with the corresponding experimental values. Under hydrostatic pressure, we find a crossover from hybridization gap to charge-transfer insulting physics due to the delicate balance of hybridization and correlations. Increasing the pressure above [Formula: see text] GPa we find a simultaneous pressure-induced volume collapse, plane-to-chain, insulator to metal transition. Finally, we have also analyzed the topology in the antiferromagnetic CaMn[Formula: see text]Bi[Formula: see text] for all pressures studied.
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UTe2 is a recently discovered unconventional superconductor that has attracted much interest because of its potentially spin-triplet topological superconductivity. Our ac calorimetry, electrical resistivity, and x-ray absorption study of UTe2 under applied pressure reveals key insights on the superconducting and magnetic states surrounding pressure-induced quantum criticality at P c1 = 1.3 GPa. First, our specific heat data at low pressures, combined with a phenomenological model, show that pressure alters the balance between two closely competing superconducting orders. Second, near 1.5 GPa, we detect two bulk transitions that trigger changes in the resistivity, which are consistent with antiferromagnetic order, rather than ferromagnetism. Third, the emergence of magnetism is accompanied by an increase in valence toward a U4+ (5f 2) state, which indicates that UTe2 exhibits intermediate valence at ambient pressure. Our results suggest that antiferromagnetic fluctuations may play a more substantial role on the superconducting state of UTe2 than previously thought.
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We report the electronic and magnetic properties of stoichiometric CeAuBi2 single crystals. At ambient pressure, CeAuBi2 orders antiferromagnetically below a Néel temperature (TN ) of 19 K. Neutron diffraction experiments revealed an antiferromagnetic propagation vector τ ^ = [ 0 , 0 , 1 ∕ 2 ] , which doubles the paramagnetic unit cell along the c axis. At low temperatures several metamagnetic transitions are induced by the application of fields parallel to the c axis, suggesting that the magnetic structure of CeAuBi2 changes as a function of field. At low temperatures, a linear positive magnetoresistance may indicate the presence of band crossings near the Fermi level. Finally, the application of external pressure favors the antiferromagnetic state, indicating that the 4f electrons become more localized.
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Topological states of matter have attracted a lot of attention recently due to their intriguing physical properties and potential applications. In particular, the family of half-Heusler compounds [Formula: see text] (R = rare earth, M = Pt, Pd or Au, and T = Bi, Sb, Pb or Sn) has been predicted to display tunable topological properties via their cubic unit cell volume and/or the charges of the M and T atoms. In this work, we report electron spin resonance (ESR), along with complementary macroscopic experiments, in the putative topologically trivial rare-earth doped (Gd, Nd and Er) YPdBi. From magnetic susceptibility data analysis constrained by ESR results, we were able to extract the fourth (A 4) and sixth (A 6) order crystal field parameters (CFP) for YPdBi and compared them with those already reported to YPtBi, which is known as a topologically non-trivial compound. We observed that the sign of the CFP changes systematically from YPdBi to YPtBi, possibly due to the inversion of the valence and conduction bands at the Fermi level. The enhanced spin-orbit coupling in YPtBi, when compared to YPdBi, induces the band inversion that drives the system to a non-trivial topological state. This band inversion likely has an effect on the effective charges surrounding the magnetic dopants that are probed by the CFP.
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SmB_{6} is a candidate topological Kondo insulator that displays surface conduction at low temperatures. Here, we perform torque magnetization measurements as a means to detect de Haas-van Alphen (dHvA) oscillations in SmB_{6} crystals grown by aluminum flux. We find that dHvA oscillations occur in single crystals containing embedded aluminum, originating from the flux used to synthesize SmB_{6}. Measurements on a sample with multiple, unconnected aluminum inclusions show that aluminum crystallizes in a preferred orientation within the SmB_{6} cubic lattice. The presence of aluminum is confirmed through bulk susceptibility measurements, but does not show a signature in transport measurements. We discuss the ramifications of our results.
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High magnetic fields induce a pronounced in-plane electronic anisotropy in the tetragonal antiferromagnetic metal CeRhIn_{5} at H^{*}â³30 T for fields ≃20° off the c axis. Here we investigate the response of the underlying crystal lattice in magnetic fields to 45 T via high-resolution dilatometry. At low fields, a finite magnetic field component in the tetragonal ab plane explicitly breaks the tetragonal (C_{4}) symmetry of the lattice revealing a finite nematic susceptibility. A modest a-axis expansion at H^{*} hence marks the crossover to a fluctuating nematic phase with large nematic susceptibility. Magnetostriction quantum oscillations confirm a Fermi surface change at H^{*} with the emergence of new orbits. By analyzing the field-induced change in the crystal-field ground state, we conclude that the in-plane Ce 4f hybridization is enhanced at H^{*}, in agreement with the in-plane lattice expansion. We argue that the nematic behavior observed in this prototypical heavy-fermion material is of electronic origin, and is driven by the hybridization between 4f and conduction electrons which carries the f-electron anisotropy to the Fermi surface.
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We report in-plane electrical resistivity studies of CeCuBi2 and LaCuBi2 single crystals under applied pressure. At ambient pressure, CeCuBi2 is a c-axis Ising antiferromagnet with a transition temperature [Formula: see text] K. In a magnetic field applied along the c-axis at [Formula: see text] K a spin-flop transition takes place [Formula: see text] T. Applying pressure on CeCuBi2 suppresses T N at a slow rate. [Formula: see text] extrapolates to zero temperature at [Formula: see text] GPa. The critical field of the spin-flop transition [Formula: see text] displays a maximum of 6.8 T at [Formula: see text] GPa. At low temperatures, a zero-resistance superconducting state emerges upon the application of external pressure having a maximum T c of 7 K at 2.6 GPa in CeCuBi2. High-pressure electrical-resistivity experiments on the non-magnetic reference compound LaCuBi2 reveal also a zero resistance state with similar critical temperatures in the same pressure range as CeCuBi2. The great similarity between the superconducting properties of both materials and elemental Bi suggests a common origin of the superconductivity. We discuss that the appearance of this zero resistance state superconductivity may be related to the Bi layers present in the crystalline structure of both compounds and, therefore, could be intrinsic to CeCuBi2 and LaCuBi2, however further experiments under pressure are necessary to clarify this issue.
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Unconventional superconductivity and magnetism are intertwined on a microscopic level in a wide class of materials. A new approach to this most fundamental and hotly debated issue focuses on the role of interactions between superconducting electrons and bosonic fluctuations at the interface between adjacent layers in heterostructures. Here we fabricate hybrid superlattices consisting of alternating atomic layers of the heavy-fermion superconductor CeCoIn_{5} and antiferromagnetic (AFM) metal CeRhIn_{5}, in which the AFM order can be suppressed by applying pressure. We find that the superconducting and AFM states coexist in spatially separated layers, but their mutual coupling via the interface significantly modifies the superconducting properties. An analysis of upper critical fields reveals that, upon suppressing the AFM order by applied pressure, the force binding superconducting electron pairs acquires an extreme strong-coupling nature. This demonstrates that superconducting pairing can be tuned nontrivially by magnetic fluctuations (paramagnons) injected through the interface.
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Samples of nanostructured ß-Ga wires were synthesized by a novel method of metallic-flux nanonucleation. Several superconducting properties were observed, revealing the stabilization of a weak-coupling type-II-like superconductor ([Formula: see text] [Formula: see text] 6.2 K) with a Ginzburg-Landau parameter [Formula: see text] = 1.18. This contrasts the type-I superconductivity observed for the majority of Ga phases, including small spheres of ß-Ga with diameters near 15 µm. Remarkably, our magnetization curves reveal a crossover field [Formula: see text], where we propose that the Abrikosov vortices are exactly touching their neighbors inside the Ga nanowires. A phenomenological model is proposed to explain this result by assuming that only a single row of vortices is allowed inside a nanowire under perpendicular applied field, with an appreciable depletion of Cooper pair density at the nanowire edges. These results are expected to shed light on the growing area of superconductivity in nanostructured materials.
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Applied pressure drives the heavy-fermion antiferromagnet CeRhIn5 toward a quantum critical point that becomes hidden by a dome of unconventional superconductivity. Magnetic fields suppress this superconducting dome, unveiling the quantum phase transition of local character. Here, we show that [Formula: see text] magnetic substitution at the Ce site in CeRhIn5, either by Nd or Gd, induces a zero-field magnetic instability inside the superconducting state. This magnetic state not only should have a different ordering vector than the high-field local-moment magnetic state, but it also competes with the latter, suggesting that a spin-density-wave phase is stabilized in zero field by Nd and Gd impurities, similarly to the case of Ce0.95Nd0.05CoIn5 Supported by model calculations, we attribute this spin-density wave instability to a magnetic-impurity-driven condensation of the spin excitons that form inside the unconventional superconducting state.
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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.
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This work reports on the dimensionality effects on the magnetic behavior of Fe3Ga4 compounds by means of magnetic susceptibility, electrical resistivity, and specific heat measurements. Our results show that reducing the Fe3Ga4 dimensionality, via nanowire shape, intriguingly modifies its electronic structure. In particular, the bulk system exhibits two transitions, a ferromagnetic (FM) transition temperature at T1 = 50 K and an antiferromagnetic (AFM) one at T2 = 390 K. On the other hand, nanowires shift these transition temperatures, towards higher and lower temperature for T1 and T2, respectively. Moreover, the dimensionality reduction seems to also modify the microscopic nature of the T1 transition. Instead of a FM to AFM transition, as observed in the 3D system, a transition from FM to ferrimagnetic (FERRI) or to coexistence of FM and AFM phases is found for the nanowires. Our results allowed us to propose the magnetic field-temperature phase diagram for Fe3Ga4 in both bulk and nanostructured forms. The interesting microscopic tuning of the magnetic interactions induced by dimensionality in Fe3Ga4 opens a new route to optimize the use of such materials in nanostructured devices.
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The change in resistance of a material in a magnetic field reflects its electronic state. In metals with weakly- or non-interacting electrons, the resistance typically increases upon the application of a magnetic field. In contrast, negative magnetoresistance may appear under some circumstances, e.g., in metals with anisotropic Fermi surfaces or with spin-disorder scattering and semimetals with Dirac or Weyl electronic structures. Here we show that the non-magnetic semimetal TaAs2 possesses a very large negative magnetoresistance, with an unknown scattering mechanism. Density functional calculations find that TaAs2 is a new topological semimetal [â¤2 invariant (0;111)] without Dirac dispersion, demonstrating that a negative magnetoresistance in non-magnetic semimetals cannot be attributed uniquely to the Adler-Bell-Jackiw chiral anomaly of bulk Dirac/Weyl fermions.
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Electron spin resonance (ESR) of diluted Nd(3+) ions in the topologically nontrivial semimetallic (TNSM) YBiPt compound is reported. The cubic YBiPt compound is a non-centrosymmetric half Heusler material which crystallizes in the F43m space group. The low temperature Nd(3+) ESR spectra showed a g-value of 2.66(4) corresponding to a Γ6 cubic crystal field Kramers' doublet ground state. Remarkably, the observed metallic and diffusive (Dysonian) Nd(3+) lineshape presented an unusual dependence with grain size, microwave power, Nd(3+) concentration and temperature. Moreover, the spin dynamic of the localized Nd(3+) ions in YBiPt was found to be characteristic of a phonon-bottleneck regime. It is claimed that, in this regime for YBiPt, phonons are responsible for mediating the diffusion of the microwave energy absorbed at resonance by the Nd(3+) ions to the thermal bath throughout the skin depth (δ ≃ µm). We argue that this is only possible because of the existence of highly mobile conduction electrons inside the skin depth of YBiPt that are strongly coupled to the phonons by spin-orbit coupling. Therefore, our unexpected ESR results point to a coexistence of metallic and insulating behaviors within the skin depth of YBiPt. This scenario is discussed in the light of the TNSM properties of this compound.
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We report a combined study of external pressure and Cu-substitution on BaFe2As2 single crystals grown by the in-flux technique. At ambient pressure, the Cu-substitution is known to suppress the spin density wave (SDW) phase in pure BaFe2As2(T(SDW) ≈ 140 K) and to induce a superconducting (SC) dome with a maximum transition temperature T(c)(max) ≃ 4.2 K. This T(c)(max) is much lower than the T(c) â¼ 15-28 K achieved in the case of Ru, Ni and Co substitutions. Such a lower T(c) is attributed to a Cu(2+) magnetic pair-breaking effect. The latter is strongly suppressed by applied pressure, as shown herein, Tc can be significantly enhanced by applying high pressures. In this work, we investigated the pressure effects on Cu(2+) magnetic pair-breaking in the BaFe(2-x)Cu(x)As2 series. Around the optimal concentration (x(opd) = 0.11), all samples showed a substantial increase of T(c) as a function of pressure. Yet for those samples with a slightly higher doping level (over-doped regime), T(c) presented a dome-like shape with maximum T(c) ≃ 8 K. Remarkably interesting, the under-doped samples, e.g. x = 0.02 display a maximum pressure induced T(c) ≃ 30 K which is comparable to the maximum T(c)'s found for the pure compound under external pressures. Furthermore, the magnetoresistance effect as a function of pressure in the normal state of the x = 0.02 sample also presented an evolution consistent with the screening of the Cu(2+) local moments. These findings demonstrate that the Cu(2+) magnetic pair-breaking effect is completely suppressed by applying pressure in the low concentration regime of Cu(2+) substituted BaFe2As2.
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The role of orbital differentiation on the emergence of superconductivity in the Fe-based superconductors remains an open question to the scientific community. In this investigation, we employ a suitable microscopic spin probe technique, namely Electron Spin Resonance (ESR), to investigate this issue on selected chemically substituted BaFe2As2 single crystals. As the spin-density wave (SDW) phase is suppressed, we observe a clear increase of the Fe 3d bands anisotropy along with their localization at the FeAs plane. Such an increase of the planar orbital content is interestingly independent of the chemical substitution responsible for suppressing the SDW phase. As a consequence, the magnetic fluctuations in combination with this particular symmetry of the Fe 3d bands are propitious ingredients for the emergence of superconductivity in this class of materials.
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The possible existence of a sign-changing gap symmetry in BaFe2As2-derived superconductors (SC) has been an exciting topic of research in the last few years. To further investigate this subject we combine Electron Spin Resonance (ESR) and pressure-dependent transport measurements to investigate magnetic pair-breaking effects on BaFe1.9M0.1As2 (M = Mn, Co, Cu, and Ni) single crystals. An ESR signal, indicative of the presence of localized magnetic moments, is observed only for M = Cu and Mn compounds, which display very low SC transition temperature (Tc) and no SC, respectively. From the ESR analysis assuming the absence of bottleneck effects, the microscopic parameters are extracted to show that this reduction of Tc cannot be accounted by the Abrikosov-Gorkov pair-breaking expression for a sign-preserving gap function. Our results reveal an unconventional spin- and pressure-dependent pair-breaking effect and impose strong constraints on the pairing symmetry of these materials.
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The Fe K x-ray absorption near edge structure of BaFe(2-x)Co(x)As(2) superconductors was investigated. No appreciable alteration in shape or energy position of this edge was observed with Co substitution. This result provides experimental support to previous ab initio calculations in which the extra Co electron is concentrated at the substitute site and do not change the electronic occupation of the Fe ions. Superconductivity may emerge due to bonding modifications induced by the substitute atom that weakens the spin-density-wave ground state by reducing the Fe local moments and/or increasing the elastic energy penalty of the accompanying orthorhombic distortion.