Heavy Fermion State Research Articles

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.

Complex magnetic ordering in the noncentrosymmetric metal PrCuGe3

We report on the successful synthesis of PrCuGe3 which crystallizes in the tetragonal BaNiSn3-type structure (space group: I4mm) with lattice parameters, a = 4.1470(2) Å and c = 10.185(3) Å. The material is characterized using dc magnetic susceptibility χ(T), ac magnetic susceptibility χac(T), isothermal magnetization M(B), specific heat Cp(T), and electrical resistivity ρ(T) measurements. PrCuGe3 undergoes a long-range ferromagnetic ordering at TC = 23 K, which is followed by another transition below Ttr = 17 K. TC has a quite small anomaly in Cp(T) and ρ(T) despite displaying large associated anomalies in both χ(T) and χac(T) and a sizable ferromagnetic ordered moment. Instead the transition at Ttr has a much larger anomaly in Cp(T) and ρ(T) but essentially no signal in χ(T) and χac(T). Such observations in PrCuGe3 are nontrivial. A Sommerfeld coefficient γ = 375 mJ/(mol K2) is extracted from specific heat which indicates a significant enhancement of the quasi-particle mass at low temperature. Hence, PrCuGe3 exemplifies a system with the coexistence of complex magnetic ordering and a putative heavy-fermion state.

Kondo effect and its destruction in heterobilayer transition metal dichalcogenides

Moiré structures, along with line-graph-based d-electron systems, represent a setting to realize flat bands. One form of the associated strong correlation physics is the Kondo effect. Here, we address the recently observed Kondo-driven heavy fermion state and its destruction in AB-stacked hetero-bilayer transition metal dichalcogenides, which can be controlled by the gate voltages. By studying an effective interacting Hamiltonian using the slave spin approach, we obtained a phase diagram with the total filling factor and the displacement field strength as the tunable parameters. In an extended range of the tunable displacement field, our numerical results show that the relative filling of the d orbital, which is associated with the highest moiré band from the MoTe2 layer, is enforced to be νd≈1 by the interaction. This agrees with the experimental observation. We also argue that the observed high coherence temperature scale could be explained by the non-negligible bandwidth of the d orbital. Our results set the stage to address the amplified quantum fluctuations that the Kondo effect may produce in these structures and new regimes that the systems open up for Kondo-destruction quantum criticality. Published by the American Physical Society 2024

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.

Two-dimensional heavy fermions in the van der Waals metal CeSiI.

Heavy-fermion metals are prototype systems for observing emergent quantum phases driven by electronic interactions1-6. A long-standing aspiration is the dimensional reduction of these materials to exert control over their quantum phases7-11, which remains a significant challenge because traditional intermetallic heavy-fermion compounds have three-dimensional atomic and electronic structures. Here we report comprehensive thermodynamic and spectroscopic evidence of an antiferromagnetically ordered heavy-fermion ground state in CeSiI, an intermetallic comprising two-dimensional (2D) metallic sheets held together by weak interlayer van der Waals (vdW) interactions. Owing to its vdW nature, CeSiI has a quasi-2D electronic structure, and we can control its physical dimension through exfoliation. The emergence of coherenthybridization of f and conduction electrons at low temperature is supported by the temperature evolution of angle-resolved photoemission and scanning tunnelling spectra near the Fermi level andby heat capacity measurements. Electrical transport measurements on few-layer flakes reveal heavy-fermion behaviour and magnetic order down to the ultra-thin regime. Our work establishes CeSiI and related materials as a unique platform for studying dimensionally confined heavy fermions in bulk crystals and employing 2D device fabrication techniques and vdW heterostructures12 to manipulate the interplay between Kondo screening, magnetic order and proximity effects.

Two-dimensional heavy fermion in a monoatomic-layer Kondo lattice YbCu2

The Kondo effect between localized f-electrons and conductive carriers leads to exotic physical phenomena. Among them, heavy-fermion (HF) systems, in which massive effective carriers appear due to the Kondo effect, have fascinated many researchers. Dimensionality is also an important characteristic of the HF system, especially because it is strongly related to quantum criticality. However, the realization of the perfect two-dimensional (2D) HF materials is still a challenging topic. Here, we report the surface electronic structure of the monoatomic-layer Kondo lattice YbCu2 on a Cu(111) surface observed by synchrotron-based angle-resolved photoemission spectroscopy. The 2D conducting band and the Yb 4f state, located very close to the Fermi level, are observed. These bands are hybridized at low-temperature, forming the 2D HF state, with an evaluated coherence temperature of about 30 K. The effective mass of the 2D state is enhanced by a factor of 100 by the development of the HF state. Furthermore, clear evidence of the hybridization gap formation in the temperature dependence of the Kondo-resonance peak has been observed below the coherence temperature. Our study provides a new candidate as an ideal 2D HF material for understanding the Kondo effect at low dimensions.

Kondo interaction in FeTe and its potential role in the magnetic order

Finding d-electron heavy fermion states has been an important topic as the diversity in d-electron materials can lead to many exotic Kondo effect-related phenomena or new states of matter such as correlation-driven topological Kondo insulator. Yet, obtaining direct spectroscopic evidence for a d-electron heavy fermion system has been elusive to date. Here, we report the observation of Kondo lattice behavior in an antiferromagnetic metal, FeTe, via angle-resolved photoemission spectroscopy, scanning tunneling spectroscopy and transport property measurements. The Kondo lattice behavior is represented by the emergence of a sharp quasiparticle and Fano-type tunneling spectra at low temperatures. The transport property measurements confirm the low-temperature Fermi liquid behavior and reveal successive coherent-incoherent crossover upon increasing temperature. We interpret the Kondo lattice behavior as a result of hybridization between localized Fe 3dxy and itinerant Te 5pz orbitals. Our observations strongly suggest unusual cooperation between Kondo lattice behavior and long-range magnetic order.

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.

Field-induced local Fermi-liquid states in the underscreened Kondo model for Eu compounds

We have studied an underscreened Kondo model for the impurity spin S=7/2S=7/2 capturing the 4f4f characteristics of a nearly divalent Eu ion. By using the numerical renormalization group method, it is shown that an unusual heavy-fermion state is induced from the underscreened spin state when a weak crystal field is introduced. It is also found that the application of the magnetic field enhances the effective mass of the heavy fermions, reflecting the field-induced level crossing of the spin states. We will discuss the mechanism of these mass enhancements in terms of a realization of the two-stage Kondo effect.

Low-Temperature Magnetic Fluctuations Investigated by 125Te-NMR on the Uranium-Based Superconductor UTe2

To investigate the static and dynamic magnetic properties on the uranium-based superconductor UTe2, we measured the NMR Knight shift K and the nuclear spin–lattice relaxation rate 1/T1 in H || a by 125Te-NMR on a 125Te-enriched single-crystal sample. 1/T1T in H || a is much smaller than 1/T1T in H || b and c, and magnetic fluctuations along each axis are derived from the 1/T1T measured in H parallel to all three crystalline axes. The magnetic fluctuations are almost identical at two Te sites and isotropic at high temperatures, but become anisotropic below 40 K, where heavy-fermion state is formed. The character of magnetic fluctuations in UTe2 is discussed with the comparison to its static susceptibility and the results on other U-based superconductors. It is considered that the magnetic fluctuations probed with the NMR measurements are determined by the magnetic properties inside the two-leg ladder formed by U atoms, which are dominated by the qa = 0 ferromagnetic fluctuations.

Magnetic and electrical properties of a heavy-fermion compound EuRh2Al8

We report the magnetic, thermodynamic, and electrical properties of ${\mathrm{EuRh}}_{2}{\mathrm{Al}}_{8}$, a Eu-based heavy fermion member in the ${\mathrm{RT}}_{2}{\mathrm{X}}_{8}$ families with an orthorhombic $Pbam$ structure. Magnetization studies reveal multiple phase transitions in the single crystals, including two successive antiferromagnetic transitions at ${T}_{N1}\ensuremath{\sim}12.5\phantom{\rule{0.16em}{0ex}}\mathrm{K}$ and ${T}_{N2}\ensuremath{\sim}8.2\phantom{\rule{0.16em}{0ex}}\mathrm{K}$. These two transitions are closely related to competing magnetic interactions in the Shastry-Sutherland lattice, which further give rise to another in-plane spin-flop transition at 1/3 of the full magnetization below 5 K when the applied magnetic field is higher than 6 T within the $ab$ plane. In addition to these, specific heat measurements in ${\mathrm{EuRh}}_{2}{\mathrm{Al}}_{8}$ demonstrate a heavy fermion state with a large Sommerfeld coefficient $\ensuremath{\gamma}=393\phantom{\rule{0.16em}{0ex}}\mathrm{mJ}\ifmmode\cdot\else\textperiodcentered\fi{}{\mathrm{mol}}^{\ensuremath{-}1}\ifmmode\cdot\else\textperiodcentered\fi{}{\mathrm{K}}^{\ensuremath{-}2}$. Electrical transport measurement shows that its resistivity exhibits a ${T}^{2}$-dependence below ${T}_{N2}$ and a robust linear $T$-dependence above ${T}_{N1}$, which is also typical of a heavy fermion metal. Our work provides fundamental physical properties of ${\mathrm{EuRh}}_{2}{\mathrm{Al}}_{8}$ and promotes understanding of the complex magnetic interactions and unusual spin correlations in the ${\mathrm{RT}}_{2}{\mathrm{X}}_{8}$ families.

Pressure-Induced Valence Transition and Heavy-Fermion State in Europium Compounds

Pressure-Induced Valence Transition and Heavy-Fermion State in Europium Compounds

Signature of Kondo hybridisation with an orbital-selective Mott phase in 4d Ca2−xSrxRuO4

AbstractThe heavy fermion state with Kondo-hybridisation (KH), usually manifested in f-electron systems with lanthanide or actinide elements, was recently discovered in several 3d transition metal compounds without f-electrons. However, KH has not yet been observed in 4d/5d transition metal compounds, since more extended 4d/5d orbitals do not usually form flat bands that supply localised electrons appropriate for Kondo pairing. Here, we report a substitution- and temperature-dependent angle-resolved photoemission study on 4d Ca2−xSrxRuO4, which shows the signature of KH. We observed a spectral weight transfer in the γ-band, reminiscent of an orbital-selective Mott phase (OSMP). The Mott localised γ-band induces the KH with an itinerant β-band, resulting in spectral weight suppression around the Fermi level. Our work demonstrates the evolution of the OSMP with possible KH among 4d electrons, and thereby expands the material boundary of Kondo physics to 4d multi-orbital systems.

Drastic change in magnetic anisotropy of UTe2 under pressure revealed by Te125 -NMR

To investigate the normal-state magnetic properties of UTe2 under pressure, we perform 125Te nuclear magnetic resonance (NMR) measurements up to 2 GPa. Below 1.2 GPa, the b-axis NMR Knight shift shows a broad maximum at the so-called T_chimax on cooling, which is consistent with the magnetization measurement under pressure. T_chimax decreases with increasing pressure and disappears at the critical pressure Pc = 1.7 GPa, above which superconductivity is destroyed. This tendency is also observed in the temperature dependence of the nuclear spin-lattice relaxation rate 1/T1. At low pressures, 1/T1 shows a conventional Fermi-liquid behavior (1/T1T = constant) at low temperatures, indicating the formation of the heavy-fermion state. Above Pc, 1/T1T follows a 1/T behavior without any crossover to the heavy-fermion state down to the lowest temperature (~3 K). In addition, the NMR signals disappear below 3~K, due to the influence of the magnetically ordered moments. From the pressure dependence of the T_chimax and Knight shift, it was found that the Fermi surface character is abruptly changed at Pc, and that superconductivity is observed only in the heavy-fermion state.

Thermal Expansion in a diluted Ce system La1–x Ce x Cu6

The thermal expansion of a diluted Ce system La1-x Ce x Cu6 for (0.6 ≤ x ≤ 1) has been measured between 10 and 150 K to reveal the change from the coherent heavy Fermion state (0.9 ≤ x ≤ 1) to the incoherent Kondo state (0 < x ≤ 0.73). The large Ce concentration x dependence of the linear thermal expansion coefficient along b-axis αb (T) suggests that the coupling between the 4f 1 electron and the lattice strain is the largest along the b-axis in the three crystallographic axes. The maximum of the magnetic contribution to the volume thermal expansion coefficient β m(T) at T = 50 K is retained in the x range of 0.6 ≤ x ≤ 1, suggesting the crystalline electric field (CEF) level for x = 1 doesn’t change by the substitution. Furthermore, the upturn in β m(T) below 25 K, which should be a precursor of the maximum at T = 2.5 K reported for x = 1, is retained when we decrease x from 1 to 0.6. Because the ground state for x = 0.6 is the incoherent Kondo state, the robustness of the maximum at T = 50 K and upturn in the current x value implies that β m(T) in 10 ≤ T ≤ 150 K is attributed to the CEF and Kondo effects rather than the formation of the heavy Fermion state.

High-field magnetization and magnetoresistance of the honeycomb Kondo lattice alloys Ce(Pt1-x Pd x )6Al3

CePt6Al3 is a rare example of the Ce-based honeycomb lattice compound. Substitution of the isovalent Pt for Pd transforms the ground state from a paramagnetic heavy-fermion state to an antiferromagnetic (AFM) ordered state. To gain insight into the role of magnetic frustration in the honeycomb Kondo lattice, we have measured the magnetization M(B) and electrical resistivity ρ(B) of Ce(Pt1-x Pd x )6Al3 (x ≤ 0.3) in pulsed magnetic fields up to 60 T. For the single crystal with x = 0, M(B) for B along the easy c axis exhibits a metamagnetic increase and ρ(B || c) bends at Bm = 28 T. Taking the temperature at a shoulder in the magnetic susceptibility χ (ल) for B ‖ c as T χm = 17 K, the ratio μB B m/K B T >χm is estimated to be 1.1. This value agrees with those reported for Ce-based paramagnetic heavy-fermion compounds with similar magnitudes of B m. With increasing x from 0 to 0.3 in polycrystalline samples, the magnitude of M(B = 60 T) at 1.4 K increases from 0.75 to 2.0 μβ/Ce, indicating the recovery of localized 4f moments by the Pd substitution for Pt. Using the data of M(B) and ρ(B) for x = 0.1, 0.2, 0.3, we constructed B-T phase diagrams, which show a trend from a small moment AFM ordered state for x = 0.1 to a large moment AFM ordered state for x = 0.3.

Mechanism for baryogenesis via feebly interacting massive particles

We present a simple mechanism which allows the simultaneous generation of the baryon asymmetry of the Universe along with its dark matter content. To this goal, we employ the out-of-equilibrium decays of heavy bath states into a feebly coupled dark matter particle and Standard Model charged fermions. These decays lead to dark matter production via the freeze-in mechanism and, assuming that they further violate $CP$, can generate a viable matter-antimatter asymmetry in the resonant regime. We illustrate this mechanism by studying a particular realization of this general scenario, where the role of the heavy bath particles is played by $SU(3)_{\text{c}}\times SU(2)_{\text{L}}$-singlet vectorlike fermions with a non-zero hypercharge and dark matter is identified with a gauge-singlet real scalar field. We show that in the context of this simple model the cosmological constraints for the dark matter abundance and the baryon asymmetry are satisfied for masses of heavy vectorlike fermion states of a few TeV, potentially within reach of the High-Luminosity Run of the Large Hadron Collider. Dark matter, in turn, is predicted to be rather light, with a mass of a few keV.

Antiferromagnetic order in the honeycomb Kondo lattice CePt6Al3 induced by Pd substitution

The cerium-based compound $\mathrm{Ce}{\mathrm{Pt}}_{6}{\mathrm{Al}}_{3}$, in which Ce atoms form a honeycomb lattice hosting magnetic frustration, has a heavy-fermion ground state. We have observed development of magnetic order in partially Pd-substituted $\mathrm{Ce}{({\mathrm{Pt}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x})}_{6}{\mathrm{Al}}_{3}$ series up to $x$ = 0.3 by the measurements of magnetic susceptibility, electrical resistivity \ensuremath{\rho}, and specific heat $C$. In the whole range of $x$, the unit cell volume remains unchanged within 0.2%, and the effective magnetic moment stays at $2.4\phantom{\rule{0.16em}{0ex}}{\ensuremath{\mu}}_{B}/\mathrm{Ce}$. For $x$ = 0.05, both $C/T$ and $\ensuremath{\rho}(T)$ jump on cooling at ${T}_{m}=1.8\phantom{\rule{0.28em}{0ex}}\mathrm{K}$. With increasing $x$ to 0.2, ${T}_{m}$ increases to 3.8 K, where $C/T$ shows a pronounced \ensuremath{\lambda}-type anomaly. Application of magnetic fields suppresses ${T}_{m}$, which is indicative of an antiferromagnetic (AFM) ordered state. Thus, a long-range AFM order is induced by the substitution of isovalent Pd for Pt in $\mathrm{Ce}{\mathrm{Pt}}_{6}{\mathrm{Al}}_{3}$ without carrier doping and chemical pressure. We attribute the emergence of AFM order in $\mathrm{Ce}{({\mathrm{Pt}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x})}_{6}{\mathrm{Al}}_{3}$ to the randomness in the spin-orbit interaction in the Pt-Pd sublattice, which weakens both the coherent Kondo effect and magnetic frustration in the honeycomb Kondo lattice.

Nanoscale heterogeneity induced by nonmagnetic Zn dopants in the quantum critical metal CeCoIn5 : In115 NQR/NMR and Co59 NMR study

Antiferromagnetism in a prototypical quantum critical metal ${\mathrm{CeCoIn}}_{5}$ is known to be induced by slight substitutions of nonmagnetic Zn atoms for In. In nominally 7% Zn-substituted ${\mathrm{CeCoIn}}_{5}$, an antiferromagnetic (AFM) state coexists with heavy fermion superconductivity. Heterogeneity of the electronic states is investigated in Zn-doped ${\mathrm{CeCoIn}}_{5}$ by means of nuclear quadrupole and magnetic resonances (NQR and NMR). Site-dependent NQR relaxation rates $1/{T}_{1}$ indicate that the AFM state is locally nucleated around Zn substituents in the matrix of a heavy fermion state, and percolates through the bulk at the AFM transition temperature ${T}_{\mathrm{N}}$. At lower temperatures, an anisotropic superconducting (SC) gap below the SC transition temperature ${T}_{\mathrm{c}}$, and the SC state permeates through the AFM regions via a SC proximity effect. Applying an external magnetic field induces a spin-flop transition near 5 T, reducing the volume of the AFM regions. Consequently, a short-ranged inhomogeneous AFM state survives and coexists with a paramagnetic Fermi liquid state at high fields.

Kondo Holes in the Two-Dimensional Itinerant Ising Ferromagnet Fe3GeTe2.

Heavy Fermion (HF) states emerge in correlated quantum materials due to the intriguing interplay between localized magnetic moments and itinerant electrons but rarely appear in 3d-electron systems due to high itinerancy of d-electrons. Here, an anomalous enhancement of Kondo screening is observed at the Kondo hole of local Fe vacancies in Fe3GeTe2 which is a recently discovered 3d-HF system featuring Kondo lattice and two-dimensional itinerant ferromagnetism. An itinerant Kondo-Ising model is established to reproduce the experimental results and provides insight into the competition between Ising ferromagnetism and Kondo screening. Our work explains the microscopic origin of the d-electron HF states in Fe3GeTe2 and inspires future studies of the enriched quantum many-body effects with Kondo holes.