Kondo Lattice System Research Articles

Anomalies in the Dirac bands in the proximity of correlated electrons.

Dirac fermions, particles with zero rest mass, are observed in topological materials and are believed to play a key role in the exotic phenomena in fundamental science and the advancement of quantum technology. Most of the topological systems studied so far are weakly correlated systems and the study of their properties in the presence of electron correlation is an interesting emerging area of research, where the electron correlation is expected to enhance the effective mass of the particles. Here, we studied the properties of Dirac bands in a non-symmorphic layered Kondo lattice system, CeAgSb2, employing high-resolution angle-resolved photoemission spectroscopy and first-principles calculations. In addition to the Dirac cones due to non-symmorphic symmetry, this material hosts Dirac fermions in the squarenet layer in the proximity of a strongly correlated Ce layer exhibiting Kondo behavior. Experimental results reveal crossings of the highly dispersive linear bands at the Brillouin zone boundary due to non-symmorphic symmetry. In addition, there are anisotropic Dirac cones constituted by the squarenet Sb 5p states forming a diamond-shaped nodal line. These Dirac bands are linear in a wide energy range with an unusually high slope. Interestingly, near the local Ce 4f bands, these bands exhibit a change in the slope akin to the formation of a 'kink' observed in other materials due to electron-phonon coupling. The emergence of such exotic properties in proximity to strongly correlated electronic states has significant implications in the study of complex quantum materials including unconventional superconductors.

Unusual spectral features in square-net based nonsymmorphic Kondo lattice system, CeCuX2 (X = As/Sb)

We study the electronic structure of a nonsymmorphic Kondo lattice system, CeCuX2 (X = As/Sb), a promising class of correlated topological materials important for advanced technology. While both the materials show Kondo behavior in their transport properties, CeCuSb2 is antiferromagnetic and no magnetic order is observed in CeCuAs2. We studied high-quality single-crystalline samples employing hard x-ray photoemission spectroscopy. The sample cleaving exposes the square-net structured pnictogen layers. The CeCuSb2 valence band indicates a highly metallic phase. The spectral intensity at the Fermi level in CeCuAs2 is weak, revealing close to semi-metallic behavior of the system. The Ce 3d spectra exhibit multiple features; the intensity of the features changes with the change in surface sensitivity of the technique, suggesting significant differences in the surface and bulk electronic structure. The bulk spectra of the Kondo system do not exhibit the typical f0-feature often observed in such materials. Instead, a distinct feature is observed at the lower binding energy side of the well-screened peak; the signature of this feature is manifested in the spectra from high-quality single-crystalline samples. This is outstanding and calls for physics beyond existing theories of correlated systems.

Thermodynamic and electrical transport properties of CeRhSb[formula omitted]Te[formula omitted] systems: Transition from Kondo insulating to the Griffiths and non-Fermi liquid states

It follows from our analysis of CeRhSb that the formation of Kondo insulator state due to the presence of the collective spin singlet state is strongly reduced by its doping with various dopants when their amount exceeds 8%–10%, regardless of whether they are substitute Ce, Rh or Sb. A wide variety of experimental results (electrical resistivity ρ, magnetic susceptibility χ, specific heat C, x-ray photoelectron spectroscopy) and theoretical investigations have convincingly demonstrated the proposed earlier scaling law χ×ρ=const. in the Kondo insulator regime, which is universal for all known Kondo insulators. We also analyze the properties of the Griffiths phase for CeRhSb when Pd substitutes Rh, or Sb is fractionally replaced by Te or Sn, whereas doping of Ce with La leads to the formation of magnetic cluster structure as a result of the Kondo hole effect. Magnetoresistance of CeRhSb as a function of the field B shows a negative B2 behavior, which is characteristic of the Kondo–lattice systems, it is also documented for various topological materials. Electrical resistivity of CeRhSb, as well as of CeRhSb1−xTex (x≤0.6) and CeRh1−xPdxSb (x≤0.04), follows ρ=ρ0−AT law between 0.4 and ∼2.5 K, which suggests a non-Fermi liquid-like behavior due to presence of the Griffiths phase.

Superconductivity beyond the Conventional Pauli Limit in High-Pressure CeSb_{2}.

We report the discovery of superconductivity at a pressure-induced magnetic quantum phase transition in the Kondo lattice system CeSb_{2}, sustained up to magnetic fields that exceed the conventional Pauli limit eightfold. Like CeRh_{2}As_{2}, CeSb_{2} is locally noncentrosymmetric around the Ce site, but the evolution of critical fields and normal state properties as CeSb_{2} is tuned through the quantum phase transition motivates a fundamentally different explanation for its resilience to applied field.

Electronic density of state in valence fluctuating kondo lattice systems studied by point-contact spectroscopy (Review article)

This article reviews our recent point-contact spectroscopy (PCS) investigation in valence fluctuating Kondo lattice systems, EuNi2P2 and Ge-substituted EuNi2(P0.8Ge0.2)2, and YbPd. A heavy fermion (HF) compound EuNi2P2 exhibits a significant valence fluctuation owing to the intermediate Eu valence of 2.5 + at low temperatures, leading to a strong hybridization between the conduction and f electrons (c–f hybridization). The electronic density of state measurements on EuNi2P2 by using PCS technique reveal that the HF behavior arises from the formation of the indirect hybridization gap with a double-peak structure near the Fermi level due to c–f hybridization. In EuNi2(P0.8Ge0.2)2, the valence fluctuation is suppressed by the Ge substitution, and the separation of the double-peak structure decreases. These suggest that the HF behavior is induced by the valence fluctuation. In YbPd, where two-dimensional (2D) layers of Yb3+ and Yb2.6+ are alternately aligned, a HF-like behavior with a large Sommerfeld coefficient appears at low temperatures in the specific heat. The PCS spectra represent a zero-bias dip structure with an asymmetric background, reproduced by the summation of two Fano curves with two different characteristic temperatures, meaning the formation of two Kondo resonance states for each Yb3+ and Yb2.6+ site. These suggest that a local coherence causes the large Sommerfeld coefficient in the 2D layers of Yb3+, which are screened by the conduction electrons provided by the valence fluctuating Yb2.6+ sites. The observed results indicate that PCS is a powerful technique for examining the variation of electronic DOS in valence fluctuating Kondo lattice systems.

One-dimensionality signature in optical conductivity of heavy-fermion CeIr3B2

In low dimensions, the combined effects of interactions and quantum fluctuations can lead to dramatically new physics distinct from that existing in higher dimensions. Here, we investigate the electronic and optical properties of CeIr$_{3}$B$_{2}$, a quasi-one-dimensional (1D) Kondo lattice system, using $ab\ initio$ calculations. The Ce atoms in the hexagonal crystal structure form 1D chains along the $c$-axis, with extremely short Ce-Ce distances. The quasi-1D nature of the crystal structure is well reflected in its electronic structure. Extremely flat bands emerge within the $ab$-plane of the Brillouin zone, yielding sharp optical transitions in the corresponding optical conductivity. Our calculations indicate that these prominent peaks in the optical conductivity provide a clear signature of quasi-1D heavy fermion systems.

Photoemission signature of the competition between magnetic order and Kondo effect in CeCoGe3

The competition between magnetic order and Kondo effect is essential for the rich physics of heavy fermion systems. Nevertheless, how such competition is manifested in the quasiparticle bands in a real periodic lattice remains elusive in spectroscopic experiments. Here we report a high-resolution photoemission study of the antiferromagnetic Kondo lattice system CeCoGe3 with a high TN1 of 21K. Our measurements reveal a weakly dispersive 4f band at the Fermi level near the Z point, arisingfrom moderate Kondo effect. The intensity of this heavy 4f band exhibits a logarithmic increase with lowering temperature and begins to deviate from this Kondo-like behavior below 25 K, just above TN1, and eventually ceases to grow below 12 K. Our work provides direct spectroscopic evidence for the competition between magnetic order and the Kondo effect in a Kondo lattice system with local-moment antiferromagnetism, indicating a distinct scenario for the microscopic coexistence and competition of these phenomena, which might be related to the real-space modulation.

Layer-resolved electronic behavior in a Kondo lattice system, CeAgAs2

We investigate the electronic structure of an antiferromagnetic Kondo lattice system CeAgAs2 employing hard x-ray photoemission spectroscopy. CeAgAs2, an orthorhombic variant of HfCuSi2 structure, exhibits antiferromagnetic ground state, Kondo like resistivity upturn and compensation of magnetic moments at low temperatures. The photoemission spectra obtained at different photon energies suggest termination of the cleaved surface at cis-trans-As layers. The depth-resolved data show significant surface-bulk differences in the As and Ce core level spectra. The As 2p bulk spectrum shows distinct two peaks corresponding to two different As layers. The peak at higher binding energy correspond to cis-trans-As layers and is weakly hybridized with the adjacent Ce layers. The As layers between Ce and Ag-layers possess close to trivalent configuration due to strong hybridization with the neighboring atoms and the corresponding feature appear at lower binding energy. Ce 3d core level spectra show multiple features reflecting strong Ce-As hybridization and strong correlation. Intense f 0 peak is observed in the surface spectrum while it is insignificant in the bulk. In addition, we observe a features at binding energy lower than the well-screened feature indicating the presence of additional interactions. This feature becomes more intense in the bulk spectra suggesting it to be a bulk property. Increase in temperature leads to a spectral weight transfer to higher binding energies in the core level spectra and a depletion of spectral intensity at the Fermi level as expected in a Kondo material. These results reveal interesting surface-bulk differences, complex interplay of intra- and inter-layer covalency, and electron correlation in the electronic structure of this novel Kondo lattice system.

Observation of Mott instability at the valence transition of f-electron system.

Mott physics plays a critical role in materials with strong electronic correlations. Mott insulator-to-metal transition can be driven by chemical doping, external pressure, temperature and gate voltage, which is often seen in transition metal oxides with 3d electrons near the Fermi energy (e.g. cuprate superconductor). In 4f-electron systems, however, the insulator-to-metal transition is mostly driven by Kondo hybridization and the Mott physics has rarely been explored in experiments. Here, by combining the angle-resolved photoemission spectroscopy and strongly correlated band structure calculations, we show that an unusual Mott instability exists in YbInCu4 accompanying its mysterious first-order valence transition. This contrasts with the prevalent Kondo picture and demonstrates that YbInCu4 is a unique platform to explore the Mott physics in Kondo lattice systems. Our work provides important insight for the understanding and manipulation of correlated quantum phenomena in the f-electron system.

Mott physics: One of main themes in quantum materials

<sec>The competition and cooperation between the itinerancy behavior and localization behavior of electrons in correlated quantum materials, known as Mott physics, is the physical mechanism behind the diverse states of many quantum materials. This article reviews the manifestation of Mott physics in various quantum materials and establishes it as one of the main themes of quantum materials. Finding and understanding its ever-changing ways of manifestation is one of the central tasks of experimental research on condensed matter physics.</sec><sec>Specifically, the filling-control route of Mott transition is illustrated by exampling the surface K-dosed Sr<sub>2</sub>IrO<sub>4</sub>, which exhibits d-wave gap, pseudogap behavior in underdoped regime, and phase separation with inhomogeneous electronic state distribution. All of these show strong resemblances to the doped cuprate superconductors, another prototypical filling-control type of Mott transition case. On the other hand, the bandwidth-control route of Mott transition could be found in NiS<sub>2–<i>x</i></sub>Se<sub><i>x</i></sub>, where its bandwidth continuously decreases with decreasing Se concentration, until it becomes an insulator. In addition, the essence of various ways of doping in iron-based superconductors is to change their bandwidths. The superconductivity shows up at intermediate bandwidth with moderate correlations, and it diminishes when the bandwidth is large and the electron correlations are weak. For heavily electron-doped iron-selenides, there is even a Mott insulator phase with strong correlations.</sec><sec>For carbon based materials, the phase transition between the antiferromagnetic insulator and superconducting state of A15 Cs<sub>3</sub>C<sub>60</sub> as the volume of fullerene anions decreases could be understood in terms of a bandwidth-control Mott transition; the insulator-superconductor transition discovered in electrically gated “magic angle” twisted-angle bilayer graphene could be understood as a filling-control Mott transition.</sec><sec>For f electron systems, the interplay between itinerancy and localization dominates the heavy fermion behavior and their ground states. The behaviors of the f electrons are demonstrated by using the angle-resolved photoemission data of CeCoIn<sub>5</sub>, whose f electron band becomes more coherent with decreasing temperature, and the c-f hybridization is thus enhanced and the band mass of conduction band continuously increases. The c-f hybridization behaviors of CeCoIn<sub>5,</sub> CeIrIn<sub>5</sub>, and CeRhIn<sub>5</sub> are compared with each other, and the differences in hybridization strength put their ground states into different regimes of the Doniach phase diagram. Similarly, the Skutterudites 4f<sup>2</sup> Kondo lattice system PrOs<sub>4</sub>Sb<sub>12</sub> and its sibling 4f<sup>1</sup> system CeOs<sub>4</sub>Sb<sub>12</sub> also have different ground states due to a slight difference in their c-f hybridization strengths.</sec>

Microstructuring YbRh2Si2 for resistance and noise measurements down to ultra-low temperatures

The discovery of superconductivity in the quantum critical Kondo-lattice system YbRh2Si2 at an extremely low temperature of 2 mK has inspired efforts to perform high-resolution electrical resistivity measurements down to this temperature range in highly conductive materials. Here we show that control over the sample geometry by microstructuring using focused-ion-beam techniques allows to reach ultra-low temperatures and increase signal-to-noise ratios (SNRs) tenfold, without adverse effects to sample quality. In five experiments we show four-terminal sensing resistance and magnetoresistance measurements which exhibit sharp phase transitions at the Néel temperature, and Shubnikov–de-Haas (SdH) oscillations between 13 T and 18 T where we identified a new SdH frequency of 0.39 kT. The increased SNR allowed resistance fluctuation (noise) spectroscopy that would not be possible for bulk crystals, and confirmed intrinsic -type fluctuations. Under controlled strain, two thin microstructured samples exhibited a large increase of from 67 mK up to 188 mK while still showing clear signatures of the phase transition and SdH oscillations. Superconducting quantum interference device-based thermal noise spectroscopy measurements in a nuclear demagnetization refrigerator down to 0.95 mK, show a sharp superconducting transition at mK. These experiments demonstrate microstructuring as a powerful tool to investigate the resistance and the noise spectrum of highly conductive correlated metals over wide temperature ranges.

Violation of Pauli-Clogston limit in the heavy-fermion superconductor CeRh2As2 : Duality of itinerant and localized 4f electrons

We theoretically propose a mechanism to understand the violation of the Pauli-Clogston limit for the upper critical field H$_{\rm c2}$ observed in the Ce bearing heavy Fermion material CeRh$_2$As$_2$ from the view point of spin singlet pairing. It is based on a duality concept, the dual simultaneous aspects of an electron: the itinerant part and localized part of quasi-particles (QPs) originated from the 4f electrons of the Ce atoms. While the itinerant QPs directly participate in forming the Cooper pairs, the localized QPs exert the internal field so as to oppose the applied field through the antiferromagnetic exchange interaction between them. This is inherent in the dense Kondo lattice system in general. We argue that this mechanism can be applied not only to the locally noncentrosymmetric material CeRh$_2$As$_2$, but also to globally inversion symmetry broken Ce-based materials such as CePt$_3$Si. Moreover, we point out that it also works for strongly Pauli limit violated spin triplet pairing systems, such as UTe$_2$.

Development of long-range phase coherence on the Kondo lattice

Despite of many efforts, we still lack a clear picture on how heavy electrons emerge and develop on the Kondo lattice. Here we introduce a key concept named the hybridization bond phase and propose a scenario based on phase correlation to address this issue. The bond phase is a gauge-invariant quantity combining two onsite hybridization fields mediated by inter-site magnetic correlations. Its probabilistic distribution decays exponentially with site distance, from which a characteristic length scale can be extracted to describe the spatial correlation of Kondo hybridizations. Our calculations show that this correlation length grows logarithmically with lowering temperature at large Kondo coupling, and reveal a precursor pseudogap state with short-range phase correlation before long-range phase coherence is developed to form the Kondo insulating (or heavy electron) state at low temperatures. This provides a potential microscopic explanation of the two-stage hybridization proposed by recent pump-probe experiment and the logarithmic scaling in the phenomenological two-fluid model. Our work offers a novel theoretical framework to describe the phase-related physics in Kondo lattice systems.

Quasiparticle characteristics of the weakly ferromagnetic Hund metal MnSi

Hund's metals are multi-orbital systems with $3d$ or $4d$ electrons exhibiting both itinerant character and local moments, and they feature Kondo-like screenings of local orbital and spin moments, with suppressed coherence temperature driven by Hund's coupling $J_H$. They often exhibit magnetic order at low temperature, but how the interaction between the Kondo-like screening and long-range magnetic order is manifested in the quasiparticle spectrum remains an open question. Here we present spectroscopic signature of such interaction in a Hund's metal candidate MnSi exhibiting weak ferromagnetism. Our photoemission measurements reveal renormalized quasiparticle bands near the Fermi level with strong momentum dependence: the ferromagnetism manifests through possibly exchange-split bands (Q1) below $T_C$ , while the spin/orbital screenings lead to gradual development of quasiparticles (Q2) upon cooling. Our results demonstrate how the characteristic spin/orbital coherence in a Hund's metal could coexist and compete with the magnetic order to form a weak itinerant ferromagnet, via quasiparticle bands that are well separated in momentum space and exhibit distinct temperature dependence. Our results imply that the competition between the spin/orbital screening and the magnetic order in a Hund's metal bears intriguing similarity to the Kondo lattice systems.

Z2 metallic spin liquid on a frustrated Kondo lattice

Metallic spin liquid has been reported in several correlated metals, but a satisfactory theoretical description is not yet available. Here we propose a potential route to realize the metallic spin liquid and construct an effective $\mathbb{Z}_2$ gauge theory with charged fractionalized excitations on the triangular Kondo lattice. This leads to a $\mathbb{Z}_2$ metallic spin liquid featured with long-lived, heavy holon excitations of spin 0 and charge $+e$ and a partially enlarged electron Fermi surface. It differs from the weak-coupling FL$^*$ state proposed earlier and may be viewed as a fractionalized heavy fermion liquid. Our theory provides a general framework to describe the metallic spin liquid in frustrated Kondo lattice systems.

Spin-polarized supercurrent through the van der Waals Kondo-lattice ferromagnet Fe3GeTe2

In the new van der Waals Kondo-lattice Fe$_3$GeTe$_2$, itinerant ferromagnetism and heavy fermionic behaviour coexist. Both the key properties of such a system namely a spin-polarized Fermi surface and a low Fermi momentum are expected to significantly alter Andreev reflection dominated transport at a contact with a superconducting electrode, and display unconventional proximity-induced superconductivity. We observed interplay between Andreev reflection and Kondo resonance at mesoscopic interfaces between superconducting Nb and Fe$_3$GeTe$_2$. Above the critical temperature ($T_c$) of Nb, the recorded differential conductance ($dI/dV$) spectra display a robust zero-bias anomaly which is described well by a characteristic Fano line shape arising from Kondo resonance. Below $T_c$, the Fano line mixes with Andreev reflection dominated $dI/dV$ leading to a dramatic, unconventional suppression of conductance at zero bias. As a consequence, an analysis of the Andreev reflection spectra within a spin-polarized model yields an anomalously large spin-polarization which is not explained by the density of states of the spin-split bands at the Fermi surface alone. The results open up the possibilities of fascinating interplay between various quantum phenomena that may potentially emerge at the mesoscopic superconducting interfaces involving Kondo lattice systems hosting spin-polarized conduction electrons.

Continuous ferromagnetic quantum phase transition on an anisotropic Kondo lattice

Motivated by the recent discovery of ferromagnetic quantum criticality in the heavy fermion compound ${\mathrm{CeRh}}_{6}{\mathrm{Ge}}_{4}$, we develop a numerical algorithm of infinite projected entangled pair states for the anisotropic ferromagnetic Kondo-Heisenberg model in two dimensions and study the ferromagnetic quantum phase transitions with varying magnetic and hopping anisotropy. Our calculations reveal a continuous ferromagnetic quantum phase transition in the large anisotropic region and first-order quantum phase transitions for smaller anisotropy. Our results highlight the importance of magnetic anisotropy on ferromagnetic quantum criticality in Kondo lattice systems and provide a possible explanation for the experimental observation in ${\mathrm{CeRh}}_{6}{\mathrm{Ge}}_{4}$ with a quasi-one-dimensional magnetic structure. Our work opens the avenue for future studies of the rich Kondo lattice physics using state-of-the-art tensor network approaches.

Observation of quantum criticality in antiferromagnetic based (Ce1Y )2Ir3Ge5 Kondo-Lattice system

• The chemical substitution dependencies of the three power law parameters have very similar behavior. • The minimum n exponent, maximum A coefficient, and ρo residual resistivity are at the same critical concentration x cr , expecting the sign for QCP in a non-Fermi Liquid (nFL) region. • Above x cr , the A values drop abruptly and the n values increase only slightly, indicating a transition from strongly to weakly correlated regime near the critical concentration x cr . We have carried out a detailed study of the (Ce 1 −x Y x ) 2 Ir 3 Ge 5 anti-ferromagnetic compounds across the entire range of substitution 0 ≤ x ≤ 0.33 and report the results of powder X-ray diffraction, magnetic susceptibility, heat capacity, and electrical resistivity measurements to exhibit the anti-ferromagnetic phase temperature ( T N ) versus substitution x phase diagram. The pure Ce 2 Ir 3 Ge 5 system indicates anti-ferromagnetic behavior below T N = 9.5 K. Substitution of Y into (Ce 1 −x Y x ) 2 Ir 3 Ge 5 compound leads to a decrease in the anti-ferromagnetic phase temperature ( T N ). Near x = 0.3, the anti-ferromagnetic transition temperature is suppressed to zero kelvin at an apparent anti-ferromagnetic quantum critical point, without the superconductivity sign, where the temperature dependence of the heat capacity and electrical resistivity in this region reveal non-Fermi Liquid behavior. The above results, for example, the suppressing of T N, maybe a new way to find low-temperature superconductivity in these compounds.

Anomalous low-temperature physical properties of the ytterbium-based Kondo-lattice compounds Yb4TGe8 ( T=Cr , Mn, Fe, Co, and Ni)

In this study, we have prepared single crystals of ytterbium-based layered compounds ${\mathrm{Yb}}_{4}T{\mathrm{Ge}}_{8}$ ($T=\mathrm{Cr}$, Mn, Fe, Co, and Ni) and investigated their magnetic, thermal, and transport properties systematically. The magnetic properties for all the five compounds show a typical behavior for the Kondo-lattice system at high temperatures and are highly anisotropic due to orbital moments in the degenerate ground state. At low temperatures, an additional magnetic correlation enhances the magnetic susceptibility, and both the heat capacity and the electrical resistivity deviate from the Fermi-liquid-like behavior. Such unconventional behaviors at low temperatures are discussed considering a contribution of strongly correlated characters in $T$ atoms to the conduction band.

Intermediate valence state in YbB4 revealed by resonant x-ray emission spectroscopy

We report the temperature dependence of the Yb valence in the geometrically frustrated compound from 12 to 300 K using resonant x-ray emission spectroscopy at the Yb transition. We find that the Yb valence, v, is hybridized between the v = 2 and v = 3 valence states, increasing from at 12 K to at 300 K, confirming that is a Kondo system in the intermediate valence regime. This result indicates that the Kondo interaction in is substantial, and is likely to be the reason why does not order magnetically at low temperature, rather than this being an effect of geometric frustration. Furthermore, the zero-point valence of the system is extracted from our data and compared with other Kondo lattice systems. The zero-point valence seems to be weakly dependent on the Kondo temperature scale, but not on the valence change temperature scale T v .