The recently proposed novel materials class called Weyl-Kondo semimetal (WKSM) is a time reversal invariant but inversion symmetry broken Kondo semimetal in which Weyl nodes are pushed to the Fermi level by the Kondo interaction. Here we explore whether CeCu$_{1+x}$As$_2$ may be a new WKSM candidate. We report on its single-crystal growth, structure determination and physical properties investigation. Previously published studies on polycrystalline samples suggest that it is indeed a Kondo semimetal, which is confirmed by our investigations on single crystals. X-ray diffraction reveals that CeCu$_{1+x}$As$_2$ crystallizes in a tetragonal centrosymmetric structure, although the inversion symmetry could still be broken locally due to partially occupied Cu sites. Chemical analysis results in an average occupation $x$ = 0.11(1). The electrical resistivity increases logarithmically with decreasing temperature, and saturates below 10 K. A Kondo temperature $T_{\mathrm{K}}$ $\approx$ 4 K is extracted from entropy, estimated from the specific heat measurements. From Hall effect experiments, a charge carrier density of $8.8 \times 10^{20}$ cm$^{-3}$ is extracted, a value characteristic of a semimetal. The magnetization shows pronounced anisotropy, with no evidence of magnetic ordering down to 0.4 K. We thus classify CeCu$_{1.11}$As$_2$ as a tetragonal Kondo semimetal with anisotropic magnetic properties, with a possibly broken inversion symmetry, thus fulfilling the necessary conditions for a WKSM state.
We present high-resolution photoemission spectroscopy studies on the Kondo resonance of the strongly-correlated Ce system CeCu$_2$Si$_2$. Exploiting the thermal broadening of the Fermi edge we analyze position, spectral weight, and temperature dependence of the low-energy 4f spectral features, whose major weight lies above the Fermi level $E_F$. We also present theoretical predictions based on the single-impurity Anderson model using an extended non-crossing approximation (NCA), including all spin-orbit and crystal field splittings of the 4f states. The excellent agreement between theory and e…
We present time-domain THz spectroscopy data of a thin film of the Kondo-lattice antiferromagnet CeCu$_2$Ge$_2$. The low frequency complex conductivity has been obtained down to temperatures below the onset of magnetic order. At low temperatures a narrow Drude-like peak forms, which is similar to ones found in other heavy fermion compounds that do not exhibit magnetic order. Using this data in conjunction with DC resistivity measurements, we obtain the frequency dependence of the scattering rate and effective mass through an extended Drude model analysis. The zero frequency limit of this analy…
We report systematic studies of CeCu$_9$In$_2$, which appears to be a new Kondo lattice system. Electrical resistivity exhibits a logarithmic law characteristic of Kondo systems with a broad maximum at $T_{coh}\approx$45 K and it obeys the Fermi liquid theory at low temperature. Specific heat of CeCu$_9$In$_2$ is well described by the Einstein and Debye models with electronic part at high temperature. Fitting of the Schottky formula to low temperature 4f contribution to specific heat yielded crystal field splitting of 50.2 K between a doublet and quasi-quartet. The Schotte-Schotte model estima…
We present an X-ray photoemission study of the heavy-fermion system CeCu$_{6-x}$Au$_x$ across the magnetic quantum phase transition of this compound at temperatures above the single-ion Kondo temperature $T_K$. In dependence of the Au concentration $x$ we observe a sudden change of the $f$-occupation number $n_f$ and the core-hole potential $U_{df}$ at the critical concentration $x_c=0.1$. We interpret these findings in the framework of the single-impurity Anderson model. Our results are in excellent agreement with findings from earlier UPS measurements %\cite{klein08qpt} and provide further i…
Single crystals of the new compound CeCu0.18Al0.24Si1.58 have been grown by high-temperature solution growth method using a eutectic Al-Si mixture as flux. This compound is derived from the binary CeSi2 (tetragonal ThSi2-type, Pearson symbol tI12, space group I41/amd) obtained by partial substitution of Si by Cu and Al atoms but showing full occupation of the Si crystal site (8e). While CeSi2 is a well-known valence-fluctuating paramagnetic compound, the CeCu0.18Al0.24Si1.58 phase orders ferromagnetically at TC = 9.3 K. At low temperatures the easy-axis of magnetization is along the a-axis, wh…
A large, strongly temperature-dependent Nernst coefficient, $ν$, is observed between $T$ = 2 K and 300 K for CeCu$_2$Si$_2$ and Ce$_{0.8}$La$_{0.2}$Cu$_2$Si$_2$. The enhanced $ν(T)$ is determined by the asymmetry of the on-site Kondo (conduction electron$-4f$ electron) scattering rate. Taking into account the measured Hall mobility, $μ_H$, the highly unusual thermopower, $S$, of these systems can be semiquantitatively described by $S(T)$ $=$ $-$$ν(T)/μ_H(T)$, which explicitly demonstrates that the thermopower originates from the local Kondo scattering process over a wide temperature range from…
The quantum critical point (QCP) in the archetypical heavy-fermion compound CeCu$_6$ doped by Au is described, accounting for the localized $4f$-electron of Ce, using realistic electronic structure calculations combined with dynamical mean-field theory (DMFT). Magnetism trends in Ce(Cu$_{1-ε}$Au$_ε$)$_6$ are compared with those in Co-doped CeCu$_{5}$, which resides on the non-ferromagnetic side of the composition space of one of the earliest rare-earth permanent magnet compounds, Ce(Co,Cu)$_5$. The construction of a realistic Doniach phase diagram shows that the system crosses over a magnetic …
We study a layered three-dimensional heterostructure in which two types of Kondo insulators are stacked alternatingly. One of them is the topological Kondo insulator SmB 6 , the other one an isostructural Kondo insulator AB 6 , where A is a rare-earth element, e.g., Eu, Yb, or Ce. We find that if the latter orders ferromagnetically, the heterostructure generically becomes a magnetic Weyl Kondo semimetal, while antiferromagnetic order can yield a magnetic Dirac Kondo semimetal. We detail both scenarios with general symmetry considerations as well as concrete tight-binding calcu-lations and show…
We present a high-resolution photoemission study on the strongly correlated Ce-compounds CeCu_6, CeCu_2Si_2, CeRu_2Si_2, CeNi_2Ge_2, and CeSi_2. Using a normalization procedure based on a division by the Fermi-Dirac distribution we get access to the spectral density of states up to an energy of 5 k_BT above the Fermi energy E_F. Thus we can resolve the Kondo resonance and the crystal field (CF) fine-structure for different temperatures above and around the Kondo temperature T_K. The CF peaks are identified with multiple Kondo resonances within the multiorbital Anderson impurity model. Our theo…
The crystal-field ground state wave function of CeCu$_2$Si$_2$ has been investigated with linear polarized $M$-edge x-ray absorption spectroscopy from 250mK to 250K, thus covering the superconducting ($T_{\text{c}}$=0.6K), the Kondo ($T_{\text{K}}$$\approx$20K) as well as the Curie-Weiss regime. The comparison with full-multiplet calculations shows that the temperature dependence of the experimental linear dichroism is well explained with a $Γ_7^{(1)}$ crystal-field ground-state and the thermal population of excited states at around 30meV. The crystal-field scheme does not change throughout th…
Heavy fermion semimetals represent a promising setting to explore topological metals driven by strong correlations. In this paper, we i) summarize the theoretical results in a Weyl-Kondo semimetal phase for a strongly correlated model with inversion-symmetry-breaking and time-reversal invariance, and the concurrent work that has experimentally discovered this phase in the non-magnetic non-centrosymmetric heavy fermion system Ce$_3$Bi$_4$Pd$_3$; and ii) describe what is expected theoretically when the time-reversal symmetry is also broken.
We consider a spin-1/2 Heisenberg chain coupled via a Kondo interaction to two-dimensional Dirac fermions. The Kondo interaction is irrelevant at the \textit{decoupled} fixed-point, leading to the existence of a Kondo-breakdown phase and a Kondo-breakdown critical point separating such a phase from a heavy Fermi liquid. We reach this conclusion on the basis of a renormalization group analysis, large-N calculations as well as extensive auxiliary-field quantum Monte Carlo simulations. We extract quantities such as the zero-bias tunneling conductance which will be relevant to future experiments i…
There is considerable interest in the intersection of correlations and topology, especially in metallic systems. Among the outstanding questions are how strong correlations drive novel topological states and whether such states can be readily controlled. Here we study the effect of a Zeeman coupling on a Weyl-Kondo semimetal in a nonsymmorphic and noncentrosymmetric Kondo-lattice model. A sequence of distinct and topologically nontrivial semimetal regimes are found, each containing Kondo-driven and Fermi-energy-bound Weyl nodes. The nodes annihilate at a magnetic field that is smaller than wha…
We study the competition between Kondo screening and frustrated magnetism on the non-symmorphic Shastry-Sutherland Kondo lattice at a filling of two conduction electrons per unit cell. A previous analysis of this model identified a set of gapless partially Kondo screened phases intermediate between the Kondo-destroyed paramagnet and the heavy Fermi liquid. Based on crystal symmetries, we argue that (i)~both the paramagnet and the heavy Fermi liquid are {\it semimetals} protected by a glide symmetry; and (ii)~partial Kondo screening breaks the symmetry, removing this protection and allowing the…
We investigate the Kondo effect of the Fermi arcs in a time-reversal-invariant Weyl semimetal with the variational method. To show the consequence brought out by the nontrivial spin texture, we calculate the spatial spin-spin correlation functions. The correlation functions exhibit high anisotropy. The diagonal correlation functions are dominated by the antiferromagnetic correlation while the off-diagonal part has more complicated pattern. The correlation functions obey the same symmetry as the spin texture. Tuning chemical potential changes the pattern of the correlation functions and the cor…
The quantum phase transition between paramagnetic and antiferromagnetic phases of the Kondo lattice model with Ising anisotropy in the intersite exchange is studied within the framework of extended dynamical mean-field theory. Nonperturbative numerical solutions at zero temperature point to a continuous transition for both two- and three-dimensional magnetism. In the former case, the transition is associated with critical local physics, characterized by a vanishing Kondo scale and by an anomalous exponent in the dynamics close in value to that measured in heavy-fermion CeCu_{5.9}Au_{0.1}.
There is considerable current interest to explore electronic topology in strongly correlated metals, with heavy fermion systems providing a promising setting. Recently, a Weyl-Kondo semimetal phase has been concurrently discovered in theoretical and experimental studies. The theoretical work was carried out in a Kondo lattice model that is time-reversal invariant but inversion-symmetry breaking. In this paper, we show in some detail how nonsymmorphic space-group symmetry and strong correlations cooperate to form Weyl nodal excitations with highly reduced velocity and pin the resulting Weyl nod…
A technique for measuring the electrical resistivity and absolute thermopower is presented for pressures up to 30 GPa, temperatures down to 25 mK and magnetic fields up to 10 T. With the examples of CeCu2Ge2 and CeCu2Si2 we focus on the interplay of normal phase and superconducting properties. With increasing pres- sure, the behaviour of CeCu2Ge2 evolves from that of an antiferromagnetically ordered Kondo system to that characteristic of an intermediate valence compound as the Kondo temperature increases by about two orders of magnitude. In the pressure window 8-10 < P < 20 GPa, a superconduct…
The observation of quantum criticality in diverse classes of strongly correlated electron systems has been instrumental in establishing ordering principles, discovering new phases, and identifying the relevant degrees of freedom and interactions. At focus so far have been insulators and metals. Semimetals, which are of great current interest as candidate phases with nontrivial topology, are much less explored in experiments. Here we study the Kondo semimetal CeRu$_4$Sn$_6$ by magnetic susceptibility, specific heat, and inelastic neutron scattering experiments. The power-law divergence of the m…
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 …
Coherent magnetic excitations in a topological Kondo semimetal
Zhejiang University（浙江大学）；ISIS Facility, STFC Rutherford Appleton Laboratory（STFC卢瑟福阿普尔顿实验室ISIS设施）；University of Johannesburg（约翰内斯堡大学）；Tokyo Metropolitan University（东京都立大学）；Indian Institute of Science（印度科学学院）；J-PARC Center（日本质子加速器研究机构中心）；Hiroshima University（广岛大学）；Institute for Advanced Study in Physics, Zhejiang University（浙江大学物理学高等研究院）；Institute of Fundamental and Transdisciplinary Research, Zheji（浙江基础与交叉研究学院）
Recent theoretical studies of topologically nontrivial electronic states in Kondo insulators have pointed to the importance of spin-orbit coupling (SOC) for stabilizing these states. However, systematic experimental studies that tune the SOC parameter $λ_{\rm{SOC}}$ in Kondo insulators remain elusive. The main reason is that variations of (chemical) pressure or doping strongly influence the Kondo coupling $J_{\text{K}}$ and the chemical potential $μ$ -- both essential parameters determining the ground state of the material -- and thus possible $λ_{\rm{SOC}}$ tuning effects have remained unnoti…
Recently the Ce-based caged-type compounds having general formula CeT2Al10 (T=Fe, Ru and Os) have generated considerable interest due to the Kondo semiconducting paramagnetic ground state (down to 40 mK) observed in CeFe2Al10 and anomalously high magnetic ordering temperature with a spin gap formation at low temperatures in Kondo semimetals CeRu2Al10 and CeOs2Al10. The formation of long-range magnetic ordering out of the Kondo semiconducting/semimetallic state itself is extraordinary and these are the first examples of this enigmatic coexistence of electronic ground states. These compounds als…
The "failed Kondo insulator" CeNiSn has long been suspected to be a nodal metal, with a node in the hybridization matrix elements. Here we carry out a series of Nernst effect experiments to delineate whether the severely anisotropic magnetotransport coefficients do indeed derive from a nodal metal or can simply be explained by a highly anisotropic Fermi surface. Our experiments reveal that despite an almost 20-fold anisotropy in the Hall conductivity, the large Nernst signal is isotropic. Taken in conjunction with the magnetotransport anisotropy, these results provide strong support for an iso…
Kondo-based semimetals and semiconductors are of extensive current interest as a viable platform for strongly correlated states. It is thus important to understand the routes towards such dilute-carrier correlated states. One established pathway is through Kondo effect in metallic non-magnetic analogues. Here we advance a new mechanism, through which Kondo-based semimetals develop out of conduction electrons with a low carrier-density in the presence of an even number of rare-earth sites. We demonstrate this effect by studying the Kondo material Yb3Ir4Ge13 along with its closed-f-shell counter…
Using angle-resolved photoemission spectroscopy (ARPES) and resonant ARPES, we report evidence of strong anisotropic conduction-f electron mixing (c-f mixing) in CeBi by observing a largely expanded Ce-5d pocket at low temperature, with no change in the Bi-6p bands. The Fermi surface (FS) expansion is accompanied by a pronounced spectral weight transfer from the local 4f 0 peak of Ce (corresponding to Ce3+) to the itinerant conduction bands near the Fermi level. Careful analysis suggests that the observed large FS change (with a volume expansion of the electron pocket up to 40%) can most natur…
We study the Kondo effect in three-dimensional (3D) Dirac materials and Weyl semimetals. We find the scaling of the Kondo temperature with respect to the doping $n$ and the coupling $J$ between the moment of the magnetic impurity and the carriers of the semimetal. We find that when the temperature is much smaller than the Kondo temperature the resistivity due to the Kondo effect scales as the $n^{-4/3}$.We also study the effect of the interplay of long-range scalar disorder and Kondo effect. In the presence of disorder-induced long-range carrier density inhomogeneities the Kondo effect is not …
Nonlinear responses give rise to various exciting phenomena, which are forbidden in linear responses. Among them, one of the most fascinating phenomena is the recently observed giant spontaneous Hall effect in $\mathrm{Ce_{3}Bi_{4}Pd_{3}}$. This material is a promising candidate for a Weyl-Kondo semimetal, and this experiment implies that strong correlation effects can enhance the nonlinear Hall effect. However, most theoretical studies on nonlinear responses have been limited to free systems, and the connection between nonlinear responses and strong correlation effects is poorly understood. M…
We theoretically study the Kondo screening of a spin-1/2 magnetic impurity in the bulk of a type-II Weyl semimetal (WSM) by use of the variational wave function method. We consider a type-II WSM model with two Weyl nodes located on the $k_z$-axis, and the tilting of the Weyl cones are along the $k_x$ direction. Due to co-existing electron and hole pockets, the density of states at the Fermi energy becomes finite, leading to a significant enhancement of Kondo effect. Consequently, the magnetic impurity and the conduction electrons always form a bound state, this behavior is distinct from that i…
Nontrivial topology in condensed matter systems enriches quantum states of matter, to go beyond either the classification into metals and insulators in terms of conventional band theory or that of symmetry broken phases by Landau's order parameter framework. So far, focus has been on weakly interacting systems, and little is known about the limit of strong electron correlations. Heavy fermion systems are a highly versatile platform to explore this regime. Here we report the discovery of a giant spontaneous Hall effect in the Kondo semimetal Ce3Bi4Pd3 that is noncentrosymmetric but preserves ti…
We demonstrate theoretically that the golden phase of SmS ($g$-SmS), a correlated mixed-valent system, exhibits nontrivial surface states with diverse topology. It turns out that this material is an ideal playground to investigate different band topologies in different surface terminations. We have explored surface states on three different (001), (111), and (110) surface terminations. Topological signature in the (001) surface is not apparent due to a hidden Dirac cone inside the bulk-projected bands. In contrast, the (111) surface shows a clear gapless Dirac cone in the gap region, demonstra…
We report experimental signatures of topological transitions among the Weyl semimetal states of pyrochlore Pr2Ir2O7, where the Kondo coupling between the Ir topological electrons and the spin-ice like orders of Pr moments plays a decisive role. The magnetic-field dependence of resistivity and the Hall conductivity exhibits a plateau and a sharp jump associated with a magnetic-field hysteresis, similar to a liquid-gas-like transition in dipolar spin ice system. Furthermore, the Kondo coupling is controlled by the hydrostatic pressure, revealing that the field-induced displacement of Weyl points…
Heavy fermion systems contain not only strong electron correlations, which promote a rich set of quantum phases, but also a large spin-orbit coupling, which tends to endow the electronic states a topological character. Kondo insulators are understood in terms of a lattice of local moments coupled to conduction electrons in a half-filled band, i.e., with a dense population of about one electron per unit cell. Here, we propose that a new class of Kondo insulator arises when the conduction-electron band is nearly empty ( or, equivalently, full ) . We demonstrated the effect through a honeycomb An…
Proximity of two different materials leads to an intricate coupling of quasiparticles so that an unprecedented electronic state is often realized at the interface. Here, we demonstrate a resonance-type many-body ground state in graphene, a non-magnetic two-dimensional Dirac semimetal, when grown on SmB6, a Kondo insulator, via thermal decomposition of fullerene molecules. This ground state is typically observed in three-dimensional magnetic materials with correlated electrons. Above the characteristic Kondo temperature of the substrate, the electron band structure of pristine graphene remains …
We have investigated the local low-energy excitations in CeRu$_4$Sn$_6$, a material discussed recently in the framework of strongly correlated Weyl semimetals, by means of Ce $M_5$ resonant inelastic x-ray scattering (RIXS). The availability of both $^2$F$_\frac{5}{2}$ and $^2$F$_\frac{7}{2}$ excitations of the Ce $4f^1$ configuration in the spectra allows for the determination of the crystal-electric field parameters that explain quantitatively the temperature dependence and anisotropy of the magnetic susceptibility. The absence of an azimuthal dependence in the spectra indicates that all cry…
We performed calculations of the electronic band structure and the Fermi surface as well as measured the longitudinal resistivity $ρ_{xx}(T,H)$, Hall resistivity $ρ_{xy}(T,H)$, and magnetic susceptibility as a function of temperature and various magnetic fields for VAs$_2$ with a monoclinic crystal structure. The band structure calculations show that VAs$_2$ is a nodal-line semimetal when spin-orbit coupling is ignored. The emergence of a minimum at around 11 K in $ρ_{xx}(T)$ measured at $H$ = 0 demonstrates that an additional magnetic impurity (V$^{4+}$, $S$ = 1/2) occurs in VAs$_2$ single cr…
We have investigated temperature-dependent behaviors of electronic structure and resistivity in a mixed-valent golden phase of SmS, based on the dynamical mean-field theory band structure calculations. Upon cooling, the coherent Sm 4$f$ bands are formed to produce the hybridization induced pseudogap near the Fermi level, and accordingly the topology of Fermi surface is changed to exhibit a Lifshitz-like transition. The surface states emerging in the bulk gap region are found to be not topologically protected states but just typical Rashba spin-polarized states, indicating that SmS is not a top…
Using angle-resolved photoemission spectroscopy (ARPES) and low-energy electron diffraction (LEED), together with density-functional theory (DFT) calculation, we report the formation of charge density wave (CDW) and its interplay with the Kondo effect and topological states in CeSbTe. The observed Fermi surface (FS) exhibits parallel segments that can be well connected by the observed CDW ordering vector, indicating that the CDW order is driven by the electron-phonon coupling (EPC) as a result of the nested FS. The CDW gap is large (~0.3 eV) and momentum-dependent, which naturally explains the…
Synergic effect of electronic correlation and spin-orbit coupling is an emerging topic in topological materials. Central to this rapidly developing area are the prototypes of strongly correlated heavy-fermion systems. Recently, some Ce-based compounds are proposed to host intriguing topological nature, among which the electronic properties of CeSb are still under debate. In this paper, we report a comprehensive study combining magnetic and electronic transport measurements, and electronic band structure calculations of this compound to identify its topological nature. Quantum oscillations are …
A theory is presented which accounts for the dynamical generation of a hybridization gap with nodes in the Kondo insulating materials $CeNiSn$ and $CeRhSb$. We show that Hunds interactions acting on virtual $4f^2$ configurations of the cerium ion can act to dynamically select the shape of the cerium ion by generating a Weiss field which couples to the shape of the ion. In low symmetry crystals where the external crystal fields are negligible, this process selects a nodal Kondo semimetal state as the lowest energy configuration.
We utilize the variational method to study the Kondo screening of a spin-$1/2$ magnetic impurity in a three-dimensional (3D) Weyl semimetal with two Weyl nodes along the $k_z$-axis. The model reduces to a 3D Dirac semimetal when the separation of the two Weyl nodes vanishes. When the chemical potential lies at the nodal point, $μ=0$, the impurity spin is screened only if the coupling between the impurity and the conduction electron exceeds a critical value. For finite but small $μ$, the impurity spin is weakly bound due to the low density of state, which is proportional to $μ^2$, contrary to t…
Topology and strong electron correlations are crucial ingredients in emerging quantum materials, yet their intersection in experimental systems has been relatively limited to date. Strongly correlated Weyl semimetals, particularly when magnetism is incorporated, offer a unique and fertile platform to explore emergent phenomena in novel topological matter and topological spintronics. The antiferromagnetic Weyl semimetal Mn3Sn exhibits many exotic physical properties such as a large spontaneous Hall effect and has recently attracted intense interest. In this work, we report synthesis of epitaxia…
Magnetic impurities in three-dimensional Dirac and Weyl systems are shown to exhibit a fascinatingly diverse range of Kondo physics, with distinctive experimental spectroscopic signatures. When the Fermi level is precisely at the Dirac point, Dirac semimetals are in fact unlikely candidates for a Kondo effect due to the pseudogapped density of states. However, the influence of a nearby quantum critical point leads to the unconventional evolution of Kondo physics for even tiny deviations in the chemical potential. Separating the degenerate Dirac nodes produces a Weyl phase: time-reversal symmet…
