Unraveling the origin of Kondo-like behavior in the 3d-electron heavy-fermion compound YFe2Ge2.

The heavy fermion (HF) state of [Formula: see text]-electron systems is of great current interest since it exhibits various exotic phases and phenomena that are reminiscent of the Kondo effect in [Formula: see text]-electron HF systems. Here, we present a combined infrared spectroscopy and first-principles band structure calculation study of the [Formula: see text]-electron HF compound YFe[Formula: see text]Ge[Formula: see text]. The infrared response exhibits several charge-dynamical hallmarks of HF and a corresponding scaling behavior that resemble those of the [Formula: see text]-electron HF systems. In particular, the low-temperature spectra reveal a dramatic narrowing of the Drude response along with the appearance of a hybridization gap ([Formula: see text] 50 meV) and a strongly enhanced quasiparticle effective mass. Moreover, the temperature dependence of the infrared response indicates a crossover around [Formula: see text] 100 K from a coherent state at low temperature to a quasi-incoherent one at high temperature. Despite of these striking similarities, our band structure calculations suggest that the mechanism underlying the HF behavior in YFe[Formula: see text]Ge[Formula: see text] is distinct from the Kondo scenario of the [Formula: see text]-electron HF compounds and even from that of the [Formula: see text]-electron iron-arsenide superconductor KFe[Formula: see text]As[Formula: see text]. For the latter, the HF state is driven by orbital-selective correlations due to a strong Hund's coupling. Instead, for YFe[Formula: see text]Ge[Formula: see text] the HF behavior originates from the band flatness near the Fermi level induced by the combined effects of kinetic frustration from a destructive interference between the direct Fe-Fe and indirect Fe-Ge-Fe hoppings, band hybridization involving Fe [Formula: see text] and Y [Formula: see text] electrons, and electron correlations. This highlights that rather different mechanisms can be at the heart of the HF state in [Formula: see text]-electron systems.

Enhanced triplet superconductivity in next-generation ultraclean UTe2.

The unconventional superconductor UTe[Formula: see text] exhibits numerous signatures of spin-triplet superconductivity-a rare state of matter which could enable quantum computation protected against decoherence. UTe[Formula: see text] possesses a complex phase landscape comprising two magnetic field-induced superconducting phases, a metamagnetic transition to a field-polarized state, along with pair- and charge-density wave orders. However, contradictory reports between studies performed on UTe[Formula: see text] specimens of varying quality have severely impeded theoretical efforts to understand the microscopic origins of the exotic superconductivity. Here, we report a comprehensive suite of high magnetic field measurements on a generation of pristine quality UTe[Formula: see text] crystals. Our experiments reveal a significantly revised high magnetic field superconducting phase diagram in the ultraclean limit, showing a pronounced sensitivity of field-induced superconductivity to the presence of crystalline disorder. We employ a Ginzburg-Landau model that excellently captures this acute dependence on sample quality. Our results suggest that in close proximity to a field-induced metamagnetic transition the enhanced role of magnetic fluctuations-that are strongly suppressed by disorder-is likely responsible for tuning UTe[Formula: see text] between two distinct spin-triplet superconducting phases.

Crystallization of heavy fermions via epitaxial strain in spinel LiV2O4 thin film.

The mixed-valent spinel LiV2O4 is known as the first oxide heavy-fermion system. There is a general consensus that a subtle interplay of charge, spin, and orbital degrees of freedom of correlated electrons plays a crucial role in the enhancement of quasi-particle mass, but the specific mechanism has remained yet elusive. A charge-ordering (CO) instability of V3+ and V4+ ions that is geometrically frustrated by the V pyrochlore sublattice from forming a long-range CO down to T = 0 K has been proposed as a prime candidate for the mechanism. Here, we uncover the hidden CO instability by applying epitaxial strain on single-crystalline LiV2O4 thin films. We find a crystallization of heavy fermions in a LiV2O4 film on MgO, where a charge-ordered insulator comprising of a stack of V3+ and V4+ layers along [001], the historical Verwey-type ordering, is stabilized by the in-plane tensile and out-of-plane compressive strains from the substrate. Our discovery of the [001] Verwey-type CO, together with previous realizations of a distinct [111] CO, evidence the close proximity of the heavy-fermion state to degenerate CO states mirroring the geometrical frustration of the V pyrochlore lattice, which supports the CO instability scenario for the mechanism behind the heavy-fermion formation.

Direct measurement of the evolution of magnetism and superconductivity toward the quantum critical point.

Nontrivial quantum states can be realized in the vicinity of the quantum critical point (QCP) in many strongly correlated electron systems. In particular, an emergence of unconventional superconductivity around the QCP strongly suggests that the quantum critical fluctuations play a central role in the superconducting pairing mechanism. However, a clear signature of the direct coupling between the superconducting pairing states and the quantum criticality has not yet been elucidated by the microscopic probes. Herein, we present muon spin rotation/relaxation and neutron diffraction measurements in the superconducting dome of CeCo(In1 - xZnx)5. It was found that a magnetically ordered state develops at x≥ 0.03, coexisting with the superconductivity. The magnitude of the ordered magnetic moment is continuously reduced with decreasing x, and it disappears below x∼ 0.03, indicating a second-order phase transition and the presence of the QCP at this critical Zn concentration. Furthermore, the magnetic penetration depth diverges toward the QCP. These facts provide evidence for the intimate coupling between quantum criticality and Cooper pairing.

Nature of the Unconventional Heavy-Fermion Kondo State in Monolayer CeSiI.

CeSiI has been recently isolated in the ultrathin limit, establishing CeSiI as the first intrinsic two-dimensional van der Waals heavy-fermion material up to 85 K. We show that, due to the strong spin-orbit coupling, the local moments develop a multipolar real-space magnetic texture, leading to local pseudospins with a nearly vanishing net moment. To elucidate its Kondo-screened regime, we extract from first-principles the parameters of the Kondo lattice model describing this material. We develop a pseudofermion methodology in combination with ab initio calculations to reveal the nature of the heavy-fermion state in CeSiI. We analyze the competing magnetic interactions leading to an unconventional heavy-fermion order as a function of the magnetic exchange between the localized f-electrons and the strength of the Kondo coupling. Our results show that the magnetic exchange interactions promote an unconventional momentum-dependent Kondo-screened phase, establishing the nature of the heavy-fermion state observed in CeSiI.

Transport gap in SmB6 protected against disorder.

The inverted resistance method was used in this study to extend the bulk resistivity of [Formula: see text] to a regime where the surface conduction overwhelms the bulk. Remarkably, regardless of the large off-stoichiometric growth conditions (inducing disorder by samarium vacancies, boron interstitials, etc.), the bulk resistivity shows an intrinsic thermally activated behavior that changes ∼7-10 orders of magnitude, suggesting that [Formula: see text] is an ideal insulator that is immune to disorder.

Sequential localization of a complex electron fluid.

Complex and correlated quantum systems with promise for new functionality often involve entwined electronic degrees of freedom. In such materials, highly unusual properties emerge and could be the result of electron localization. Here, a cubic heavy fermion metal governed by spins and orbitals is chosen as a model system for this physics. Its properties are found to originate from surprisingly simple low-energy behavior, with 2 distinct localization transitions driven by a single degree of freedom at a time. This result is unexpected, but we are able to understand it by advancing the notion of sequential destruction of an SU(4) spin-orbital-coupled Kondo entanglement. Our results implicate electron localization as a unified framework for strongly correlated materials and suggest ways to exploit multiple degrees of freedom for quantum engineering.

Weyl-Kondo semimetal in heavy-fermion systems.

Insulating states can be topologically nontrivial, a well-established notion that is exemplified by the quantum Hall effect and topological insulators. By contrast, topological metals have not been experimentally evidenced until recently. In systems with strong correlations, they have yet to be identified. Heavy-fermion semimetals are a prototype of strongly correlated systems and, given their strong spin-orbit coupling, present a natural setting to make progress. Here, we advance a Weyl-Kondo semimetal phase in a periodic Anderson model on a noncentrosymmetric lattice. The quasiparticles near the Weyl nodes develop out of the Kondo effect, as do the surface states that feature Fermi arcs. We determine the key signatures of this phase, which are realized in the heavy-fermion semimetal Ce3Bi4Pd3 Our findings provide the much-needed theoretical foundation for the experimental search of topological metals with strong correlations and open up an avenue for systematic studies of such quantum phases that naturally entangle multiple degrees of freedom.

Pressure-tuned quantum criticality in the antiferromagnetic Kondo semimetal CeNi2-δAs2.

The easily tuned balance among competing interactions in Kondo-lattice metals allows access to a zero-temperature, continuous transition between magnetically ordered and disordered phases, a quantum-critical point (QCP). Indeed, these highly correlated electron materials are prototypes for discovering and exploring quantum-critical states. Theoretical models proposed to account for the strange thermodynamic and electrical transport properties that emerge around the QCP of a Kondo lattice assume the presence of an indefinitely large number of itinerant charge carriers. Here, we report a systematic transport and thermodynamic investigation of the Kondo-lattice system CeNi2-δAs2 (δ ≈ 0.28) as its antiferromagnetic order is tuned by pressure and magnetic field to zero-temperature boundaries. These experiments show that the very small but finite carrier density of ~0.032 E-/formular unit in CeNi2-δAs2 leads to unexpected transport signatures of quantum criticality and the delayed development of a fully coherent Kondo-lattice state with decreasing temperature. The small carrier density and associated semimetallicity of this Kondo-lattice material favor an unconventional, local-moment type of quantum criticality and raises the specter of the Nozières exhaustion idea that an insufficient number of conduction-electron spins to separately screen local moments requires collective Kondo screening.

Fermi surface reconstruction and multiple quantum phase transitions in the antiferromagnet CeRhIn5.

Conventional, thermally driven continuous phase transitions are described by universal critical behavior that is independent of the specific microscopic details of a material. However, many current studies focus on materials that exhibit quantum-driven continuous phase transitions (quantum critical points, or QCPs) at absolute zero temperature. The classification of such QCPs and the question of whether they show universal behavior remain open issues. Here we report measurements of heat capacity and de Haas-van Alphen (dHvA) oscillations at low temperatures across a field-induced antiferromagnetic QCP (Bc0 ≈ 50 T) in the heavy-fermion metal CeRhIn5. A sharp, magnetic-field-induced change in Fermi surface is detected both in the dHvA effect and Hall resistivity at B0* ≈ 30 T, well inside the antiferromagnetic phase. Comparisons with band-structure calculations and properties of isostructural CeCoIn5 suggest that the Fermi-surface change at B0* is associated with a localized-to-itinerant transition of the Ce-4f electrons in CeRhIn5. Taken in conjunction with pressure experiments, our results demonstrate that at least two distinct classes of QCP are observable in CeRhIn5, a significant step toward the derivation of a universal phase diagram for QCPs.

Quantum critical behavior in heavy electron materials.

Quantum critical behavior in heavy electron materials is typically brought about by changes in pressure or magnetic field. In this paper, we develop a simple unified model for the combined influence of pressure and magnetic field on the effectiveness of the hybridization that plays a central role in the two-fluid description of heavy electron emergence. We show that it leads to quantum critical and delocalization lines that accord well with those measured for CeCoIn5, yields a quantitative explanation of the field and pressure-induced changes in antiferromagnetic ordering and quantum critical behavior measured for YbRh2Si2, and provides a valuable framework for describing the role of magnetic fields in bringing about quantum critical behavior in other heavy electron materials.

Direct evidence for a magnetic f-electron-mediated pairing mechanism of heavy-fermion superconductivity in CeCoIn5.

To identify the microscopic mechanism of heavy-fermion Cooper pairing is an unresolved challenge in quantum matter studies; it may also relate closely to finding the pairing mechanism of high-temperature superconductivity. Magnetically mediated Cooper pairing has long been the conjectured basis of heavy-fermion superconductivity but no direct verification of this hypothesis was achievable. Here, we use a novel approach based on precision measurements of the heavy-fermion band structure using quasiparticle interference imaging to reveal quantitatively the momentum space (k-space) structure of the f-electron magnetic interactions of CeCoIn5. Then, by solving the superconducting gap equations on the two heavy-fermion bands Ek(α,ß) with these magnetic interactions as mediators of the Cooper pairing, we derive a series of quantitative predictions about the superconductive state. The agreement found between these diverse predictions and the measured characteristics of superconducting CeCoIn5 then provides direct evidence that the heavy-fermion Cooper pairing is indeed mediated by f-electron magnetism.

Emergence of superconductivity in heavy-electron materials.

Although the pairing glue for the attractive quasiparticle interaction responsible for unconventional superconductivity in heavy-electron materials has been identified as the spin fluctuations that arise from their proximity to a magnetic quantum critical point, there has been no model to describe their superconducting transition at temperature Tc that is comparable to that found by Bardeen, Cooper, and Schrieffer (BCS) for conventional superconductors, where phonons provide the pairing glue. Here we propose such a model: a phenomenological BCS-like expression for Tc in heavy-electron materials that is based on a simple model for the effective range and strength of the spin-fluctuation-induced quasiparticle interaction and reflects the unusual properties of the heavy-electron normal state from which superconductivity emerges. We show that it provides a quantitative understanding of the pressure-induced variation of Tc in the "hydrogen atoms" of unconventional superconductivity, CeCoIn5 and CeRhIn5, predicts scaling behavior and a dome-like structure for Tc in all heavy-electron quantum critical superconductors, provides unexpected connections between members of this family, and quantifies their variations in Tc with a single parameter.

High-pressure synthesis and characterizations of a new ternary Ce-based compound Ce3TiAs5.

We report the structure and properties of a new Ce-based compound Ce3TiAs5synthesized under high-pressure and high-temperature conditions. It crystallizes in a hexagonal Hf5Sn3Cu-anti type structure with zig-zag like Ce chains along thecaxis. This compound is metallic and undergoes a magnetic phase transition atTN= 13 K. A metamagnetic transition occurs at ∼0.7 T. The Sommerfeld coefficient for the compound is determined to be about 215 mJ/(Ce-mol*K2), demonstrating a heavy Fermion behavior. The resistivity is featured with two humps, which arises from the synergistic effect of crystal electric field and magnetic scattering. The magnetic ordering temperatureTNgradually increases in the sequence of Ce3TiPn5with Pn = Bi, Sb, and As, which implies that the Ruderman-Kittel-Kasuya-Yosida interaction should be still predominant in Ce3TiAs5.

Effect of Ni Doping on the Thermoelectric Properties of YbCo2Zn20.

Thermoelectric devices are both solid-state heat pumps and energy generators. Having a reversible process without moving parts is of high importance for applications in remote locations or under extreme conditions. Yet, most thermoelectric devices have a rather limited energy conversion efficiency due to the natural competition between high electrical conductivity and low thermal conductivity, both being essential conditions for achieving a high energy conversion efficiency. Heavy-fermion compounds YbT2Zn20 (T = Co, Rh, Ir) have been reported to be potential candidate materials for thermoelectric applications at low temperatures. Motivated by this result, we applied chemical substitution studies on the transition metal site in order to optimize the charge carrier concentration as well as promote more efficient phonon scatterings. Here, we present the latest investigation on the Ni-doped specimens YbCo2-xNixZn20, where enhanced thermoelectric figure of merit values have been obtained.

Superconductivity in Ce-based cage compounds.

Cerium-based ternary compounds CeNi2Cd20and CePd2Cd20do not exhibit long-range order down to millikelvin temperature range. Given the large separation between Ce ions which significantly reduces the super-exchange interactions and vanishingly small Ruderman-Kittel-Kasuya-Yosida interaction, here we show that nodal superconductivity mediated by the valence fluctuations must be a ground state in these materials. We propose that the critical temperature for the superconducting transition can be significantly increased by applying hydrostatic pressure. We employ an extended periodic Anderson lattice model which includes the long-range Coulomb interactions between the itinerant electrons as well as the local Coulomb interaction between the predominantly localized and itinerant electrons to compute a critical temperature of the superconducting transition. Using the slave-boson approach we show that fluctuations mediated by the repulsive electron-electron interactions lead to the emergence ofd-wave superconductivity.

Vanishing RKKY interactions in Ce-based cage compounds.

We report the results of thermodynamic measurements in external magnetic field of the cubic Ce-based cage compounds CeT2Cd20(T= Ni,Pd). Our analysis of the heat-capacity data shows that the Γ7doublet is the ground state multiplet of the Ce3+ions. Consequently, for the Γ7doublet it can be theoretically shown that the Ruderman-Kittel-Kasuya-Yosida interaction between the localized Ce moments mediated by the conduction electrons, must vanish at temperatures much lower than the energy separating the ground state doublet from the first excited Γ8quartet. Our findings provide an insight as to why no long range order has been observed in these compounds down to temperatures in the milliKelvin range.

Nonlocal Kondo effect and two-fluid picture revealed in an exactly solvable model.

Understanding the nature of local-itinerant transition of strongly correlated electrons is one of the central problems in condensed matter physics. Heavy fermion systems describe the f-electron delocalization through Kondo interactions with conduction electrons. Tremendous efforts have been devoted to the so-called Kondo-destruction scenario, which predicts a dramatic local-to-itinerant quantum phase transition of f-electrons at zero temperature. On the other hand, two-fluid behaviors have been observed in many materials, suggesting coexistence of local and itinerant f-electrons over a broad temperature range but lacking a microscopic theoretical description. To elucidate this fundamental issue, here we propose an exactly solvable Kondo-Heisenberg model in which the spins are defined in the momentum space and the k-space Kondo interaction corresponds to a highly nonlocal spin scattering in the coordinate space. Its solution reveals a continuous evolution of the Fermi surfaces with Kondo interaction and two-fluid behaviors similar to those observed in real materials. The electron density violates the usual Luttinger's theorem, but follows a generalized one allowing for partially enlarged Fermi surfaces due to partial Kondo screening in the momentum space. Our results highlight the consequence of nonlocal Kondo interaction relevant for strong quantum fluctuation regions and provide important insight into the microscopic description of two-fluid phenomenology in heavy fermion systems.

Unusually strong electronic correlation and field-induced ordered phase in YbCo2.

We report the first study of electrical resistivity, magnetization, and specific heat on YbCo2. The measurements on a single-phased sample of YbCo2bring no evidence of magnetic ordering down to 0.3 K in a zero magnetic field. The manifestations of low Kondo temperature are observed. The specific heat value divided by temperature,C/T, keeps increasing logarithmically beyond 7 J/mol K2with decreasing temperature down to 0.3 K without no sign of magnetic ordering, suggesting a very large electronic specific heat. Analysis of the magnetic specific heat indicates that the large portion of the low-temperature specific heat is not explained simply by the low Kondo temperature but is due to the strong intersite magnetic correlation in both the 3dand 4felectrons. Temperature-dependent measurements under static magnetic fields up to 7 T are carried out, which show the evolution of field-induced transition above 2 T. The transition temperature increases with increasing field, pointing to a ferromagnetic character. The extrapolation of the transition temperature to zero field suggests that YbCo2is in the very proximity of the quantum critical point. These results indicate that in the unique case of YbCo2, the itinerant electron magnetism of Co 3d-electrons and the Kondo effect within the vicinity of quantum criticality of Yb 4f-local moments can both play a role.

Influence of Anomalous Changes in the Crystal Structure on the Transport Properties of YbNi1-xCuxAl Series of Alloys.

Results of the transport properties of the YbNi1-xCuxAl (x = 0, 0.2, 0.5, 0.8 and 1.0) series of alloys are reported. The previous analysis of X-ray diffraction patterns indicates that all compounds crystallize in the hexagonal ZrNiAl structure with a linear behavior of the unit cell volume as a function of the Cu concentration (x). This is not found in the unit cell parameters, showing a discontinuity between x = 0.5 and 0.8. Such discontinuities affect the behavior of the electrical resistivity, in which the position of the minimum temperature changes from 95 K to 175 K, and a rise in the low temperature slope in the magnetic contribution (with -lnT dependence) from 21 µΩcm to 212 µΩcm is observed. In addition, the electronic coefficient of the specific heat increases almost twofold from 125 mJ/mol·K2 (x = 0.5) to 246 mJ/mol·K2 (x = 0.8). These changes are attributed to the variation of the distance between Yb and transition metals (Ni and Cu) along the series and the different electronic properties of the transition metals (Ni and Cu).