We demonstrate that a theoretical framework fully incorporating intra-atomic correlations and multiplet structure of the localized 4f states is required in order to capture the essential physics of rare-earth semiconductors and semimetals. We focus in particular on the rare-earth semimetal erbium arsenide (ErAs), for which effective one-electron approaches fail to provide a consistent picture of both high and low-energy electronic states. We treat the many-body states of the Er 4f shell within an atomic approximation in the framework of dynamical mean-field theory. Our results for the magnetic-field dependence of the 4f local moment, the influence of multiplets on the photoemission spectrum, and the exchange splitting of the Fermi surface pockets as measured from Shubnikov-de Haas oscillations, are found to be in good agreement with experimental results.
Disorder in Weyl semimetals and superconductors is surprisingly subtle, attracting attention and competing theories in recent years. In this brief review, we discuss the current theoretical understanding of the effects of short-ranged, quenched disorder on the low energy-properties of three-dimensional, topological Weyl semimetals and superconductors. We focus on the role of non-perturbative rare region effects on destabilizing the semimetal phase and rounding the expected semimetal-to-diffusive metal transition into a cross over. Furthermore, the consequences of disorder on the resulting natu…
We numerically study the effect of short ranged potential disorder on massless noninteracting three-dimensional Dirac and Weyl fermions, with a focus on the question of the proposed quantum critical point separating the semimetal and diffusive metal phases. We determine the properties of the eigenstates of the disordered Dirac Hamiltonian ($H$) and exactly calculate the density of states (DOS) near zero energy, using a combination of Lanczos on $H^2$ and the kernel polynomial method on $H$. We establish the existence of two distinct types of low energy eigenstates contributing to the disordere…
Magnetic topological semimetals have attracted intense attention recently since these materials carry a great promise for potential applications in novel spintronic devices. Here, we report an intimate interplay between lattice, Eu magnetic order and topological semimetallic behavior in Eu$_{1-x}$Sr$_{x}$MnSb$_{2}$ driven by nonmagnetic Sr doping on magnetic Eu site. Different types of Eu spin reorientations are controllable by the Sr concentration, temperature or magnetic field, and coupled to the quantum transport properties of Dirac fermions generated by the 2D Sb layers. Our study opens a …
We study structural and magnetic properties of rare-earth based semimetals RAuGe (R = Y, Gd-Tm, and Lu) using flux-grown single crystals. These compounds belong to the noncentrosymmetric polar space group P63mc. We confirm the systematic structural evolution at room temperature as a function of ionic radius of rare earths to clarify the isopointal crossover between two polar structures: three-dimensional LiGaGe-type and quasi-two-dimensional NdPtSb-type. Magnetism shows a characteristic anisotropy in reasonable agreement with the crystal electric field (CEF) theory; the easy-plane-type anisotr…
The acute sensitivity of the electrical resistance of certain systems to magnetic fields known as extreme magnetoresistance (XMR) has recently been explored in a new materials context with topological semimetals. Exemplified by WTe$_{2}$ and rare earth monopnictide La(Sb,Bi), these systems tend to be non-magnetic, nearly compensated semimetals and represent a platform for large magnetoresistance driven by intrinsic electronic structure. Here we explore electronic transport in magnetic members of the latter family of semimetals and find that XMR is strongly modulated by magnetic order. In parti…
We review the cubic rare-earth boride series which displays diverse electronic states like localized 4f electron multiplets split by the crystal electric field (CEF), itinerant heavy-fermion quasiparticle bands of the Kondo lattice as well as gapped Kondo insulator or mixed-valent semiconductor states. Fairly exotic states may appear due to the 'hidden' order of multipoles carried by degenerate CEF multiplets, in addition to magnetic order present in many RB6 (R = rare earth) compounds. Most prominent are CeB6 and its La-diluted alloys which exhibit antiferro-quadrupolar and octupolar ordering…
We have investigated magneto-transport properties in a single crystal of pyrochore-type Nd2Ir2O7. The metallic conduction is observed on the antiferromagnetic domain walls of the all-in all-out type Ir-5d moment ordered insulating bulk state, that can be finely controlled by external magnetic field along [111]. On the other hand, an applied field along [001] induces the bulk phase transition from insulator to semimetal as a consequence of the field-induced modification of Nd-4f and Ir-5d moment configurations. A theoretical calculation consistently describing the experimentally observed featur…
Weyl semimetals have been intensely studied as a three dimensional realization of a Dirac-like excitation spectrum where the conduction bands and valence bands touch at isolated Weyl points in momentum space. Like in graphene, this property entails various peculiar electronic properties. However, recent theoretical studies have suggested that resonant scattering from rare regions can give rise to a non-zero density of states even at charge neutrality. Here, we give a detailed account of this effect and demonstrate how the semimetallic nature is suppressed at the lowest scales. To this end, we …
We report a comprehensive investigation of the structural, magnetic, transport and thermodynamic properties of a single crystal PrAlSi, in comparison to its nonmagnetic analogue LaAlSi. PrAlSi exhibits a ferromagnetic transition at $T_C$ = 17.8 K which, however, is followed by two weak phase transitions at lower temperatures. Based on the combined dc and ac magnetic susceptibility measurements, we propose the two reentrant magnetic phases below $T_C$ to be spin glasses or ferromagnetic cluster glasses. When the magnetic glassy states are suppressed by small field, several remarkable features a…
Realizing quantum materials in few atomic layer morphologies is a key to both observing and controlling a wide variety of exotic quantum phenomena. This includes topological electronic materials, where the tunability and dimensionality of few layer materials have enabled the detection of $Z_2$, Chern, and Majorana phases. Here, we report the development of a platform for thin film correlated, topological states in the magnetic rare-earth monopnictide ($RX$) system GdBi synthesized by molecular beam epitaxy. This material is known from bulk single crystal studies to be semimetallic antiferromag…
Lifshitz transition (LT) refers to an abrupt change in the electronic structure and Fermi surface, and is associated to a variety of emergent quantum phenomena. Amongst the LTs observed in known materials, the field-induced LT has been rare and its origin remains elusive. To understand the origin of field-induced LT, it is important to extend the material basis beyond the usual setting of heavy fermion metals. Here, we report on a field-induced LT in PrAlSi, a magnetic Weyl semimetal candidate with localized 4$f$ electrons, through a study of magnetotransport up to 55 T. The quantum oscillatio…
The crystal field parameters of 13 trivalent lanthanide ions substituted for La in LaF$_3$ were calculated using the combination of the band structure and Wannier function calculations. Performing an atomic exact diagonalization with thus obtained crystal-field parameters we compute the crystal-field splitting of atomic multiplets. The calculation is compared with the available experimental results and a good agreement is found.
ZrSiS-type materials represent a large material family with unusual coexistence of topological nonsymmorphic Dirac fermions and nodal-line fermions. As a special group of ZrSiS-family, LnSbTe (Ln = Lanthanide rare earth) compounds provide a unique opportunity to explore new quantum phases due to the intrinsic magnetism induced by Ln. Here we report the single crystal growth and characterization of NdSbTe, a previously unexplored LnSbTe compound. NdSbTe has an antiferromagnetic ground state with field-driven metamagnetic transitions similar to other known LnSbTe, but exhibits distinct enhanced …
Dirac semimetals show nontrivial physical properties and can host exotic quantum states like Weyl semimetals and topological insulators under suitable external conditions. Here, by combining angle-resolved photoemission spectroscopy measurements (ARPES) and first-principle calculations, we demonstrate that Zintl-phase compound SmMg$_2$Bi$_2$ belongs to the close proximity to a topological Dirac semimetallic state. ARPES results show a Dirac-like band crossing at the zone-center near the Fermi level ($E_\mathrm {F}$) which is further confirmed by first-principle calculations. Theoretical studie…
Using the recently developed method we calculate the crystal field parameters in yttrium and lutetium aluminum garnets doped with seven trivalent Kramers rare-earth ions. We then insert calculated parameters into the atomic-like Hamiltonian taking into account the electron-electron, spin-orbit and Zeeman interactions and determine the multiplet splitting by the crystal field as well as magnetic $\hat{g}$ tensors. We compare calculated results with available experimental data.
Magnetic topological materials are a class of compounds with the underlying interplay of nontrivial band topology and magnetic spin configuration. Extensive interests have been aroused due to their application potential involved with an array of exotic quantum states. With angle-resolved photoemission spectroscopy and first-principles calculations, here we study the electronic properties of two magnetic Weyl semimetal candidates PrAlSi and SmAlSi. Though the two compounds harbor distinct magnetic ground states (ferromagnetic and antiferromagnetic for PrAlSi and SmAlSi, respectively) and 4$f$ s…
Combining magnetism with band topology provides various novel phases that are otherwise impossible. Among several cases, noncollinear metallic antiferromagnets can reveal particularly rich topological physics due to their diverse magnetic ground states. However, there are only a few experimental studies due to the lack of suitable materials, especially with triangular lattice antiferromagnets. Here, we report that metallic triangular antiferromagnet Co1/3TaS2 exhibits a substantial anomalous Hall effect (AHE) related to its noncollinear magnetic order. Our first-principles calculations found t…
We study three-dimensional Dirac fermions with weak finite-range scalar potential disorder. In the clean system, the density of states vanishes quadratically at the Dirac point. Disorder is known to be perturbatively irrelevant, and previous theoretical work has assumed that the Dirac semimetal phase, characterized by a vanishing density of states, survives at weak disorder, with a finite disorder phase transition to a diffusive metal with a non-vanishing density of states. In this paper we show that nonperturbative effects from rare regions, which are missed by conventional disorder-averaged …
The ZrSiS family of compounds hosts various exotic quantum phenomena due to the presence of both topological nonsymmorphic Dirac fermions and nodal-line fermions. In this material family, the LnSbTe (Ln= lanthanide) compounds are particularly interesting owing to the intrinsic magnetism from magnetic Ln which leads to new properties and quantum states. In this work, the authors focus on the previously unexplored compound SmSbTe. The studies reveal a rare combination of a few functional properties in this material, including antiferromagnetism with possible magnetic frustration, electron correl…
We carried out inelastic neutron scattering to study the spin-orbital (SO) exciton in a single crystal sample of CoTiO$_3$ as a function of temperature. CoTiO$_3$ is a honeycomb magnet with dominant XY-type magnetic interaction and an A-type antiferromagnetic order below $\mathrm{T_N} \approx 38$~K. We found that the SO exciton becomes softer, but acquires a larger bandwidth in the paramagnetic phase, compared to that in the magnetically ordered phase. Moreover, an additional mode is only observed in the intermediate temperature range, as the sample is warmed up above the lowest accessible tem…
Dirac and Weyl semimetals provide a new example of three-dimensional electron gases which are sensitive to strong magnetic fields. In this paper we address their collective excitations in the extreme quantum limit in which the Hamiltonian can be projected to the $N=0$ Landau level. We show that the energy of the plasmon collective mode is not shifted by interactions, even though the quasiparticle bands are strongly renormalized, and that both optical and acoustic magnetoplasmons emerge from the particle-hole continuum when the chemical potential is not at the band-crossing point. The rare pres…
The Weyl semimetal MoTe$_2$ offers a rare opportunity to study the interplay between Weyl physics and superconductivity. Recent studies have found that Se substitution can boost the superconductivity up to 1.5K, but suppress the Td structure phase that is essential for the emergence of Weyl state. A microscopic understanding of possible coexistence of enhanced superconductivity and the Td phase has not been established so far. Here, we use scanning tunneling microscopy (STM) to study a optimally doped new superconductor MoTe$_{1.85}$Se$_{0.15}$ with bulk Tc ~ 1.5K. By means of quasiparticle in…
In rare-earth semiconductors, wide ligand $p$ and rare-earth 5$d$ bands coexist with localized, partially filled 4$f$ shells. A simultaneous description for both extended and localized states represents a significant challenge for first-principles theories. Here, we combine an {\it ab initio} dynamical mean-field theory approach to strong local correlations with a perturbative application of the semi-local modified Becke-Johnson exchange potential to correct the semiconducting gap. We apply this method to calculate the electronic structure and optical response of the light rare-earth sesquioxi…
The electronic structures of rare-earth elements in the HCP structure, and Europium in the BCC structure, are calculated by use of density-functional theory, DFT. Simulation of X-ray photoemission spectroscopy (XPS) and bremsstrahlung isochromatic spectroscopy (BIS) are made within DFT by imposing that f-electrons are excited by a large photon energy, either by removing from the occupied states in XPS, or by adding to the unoccupied f-states in BIS. The results show sizable differences in the apparent position of the f-states compared to the f-band energy of the ground states. This result is f…
$\mathsf{Mn_{3}Sn}$ has recently attracted considerable attention as a magnetic Weyl semimetal exhibiting concomitant transport anomalies at room temperature. The topology of the electronic bands, their relation to the magnetic ground state and their nonzero Berry curvature lie at the heart of the problem. The examination of the full magnetic Hamiltonian reveals otherwise hidden aspects of these unusual physical properties. Here, we report the full spin wave spectra of $\mathsf{Mn_{3}Sn}$ measured over a wide momentum - energy range by the inelastic neutron scattering technique. Using a linear…
Design Principles for Quasi-Isotropic Exchange in Rare-Earth Quantum Magnets
The University of Tokyo（东京大学）；Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室）；Oak Ridge National Laboratory（橡树岭国家实验室）；University of Tennessee, Knoxville（田纳西大学诺克斯维尔分校）
The Crystalline Electric Field (CEF) influence is usually described by considering an ideally symmetrical rare-earth site. In the case of cage compounds, ample excursions of the rare-earth inside the cage require an adapted CEF description. A corrective, position dependent, CEF term accounts for the deviation from the perfect symmetry. In the paramagnetic range, a CEF level with orbital degeneracy thus acquires a width reflecting the rare-earth spatial distribution. In the case, frequent in cubic systems, of an orbitally degenerate CEF ground state at the center, this width introduces an addit…
The electronic structure of the rare-earth mononitrides LnN (where Ln=rare-earth), which are promising materials for future spintronics applications, is difficult to resolve experimentally due to a strong influence of defects on their transport and optical properties. At the same time, LnN are challenging for theory, since wide semiconducting/semimetallic 2p and 5d bands need to be described simultaneously with strongly correlated 4f states. Here, we calculate the many-body spectral functions and optical gaps of a series of LnN (with Ln= Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er) by a density-functional+…
We studied the electronic structure of rare-earth ditelluride (ReTe_2 : Re = La, Pr, Sm, and Gd) using photoemission spectroscopy. From the x-ray photoelectron spectroscopy (XPS) study of the 3d core levels of rare-earth elements, we found that all the rare earth elements are trivalent. We have also made theoretical calculations using the Gunnarsson and Schoenhammer approximation and multiplet calculations for the rare earth elements to find that the La and Gd~3d peaks are well explained using our calculations. There is no considerable change in the line-shape of the Te~3d peaks depending on d…
We review recent studies of spin dynamics in rare-earth orthorhombic perovskite oxides of the type $RM$O$_3$, where $R$ is a rare-earth ion and $M$ is a transition-metal ion, using single-crystal inelastic neutron scattering (INS). After a short introduction to the magnetic INS technique in general, the results of INS experiments on both transition-metal and rare-earth subsystems for four selected compounds (YbFeO$_3$, TmFeO$_3$, YFeO$_3$, YbAlO$_3$) are presented. We show that the spectrum of magnetic excitations consists of two types of collective modes that are well separated in energy: gap…
We performed resonant soft X-ray diffraction on known charge density wave (CDW) compounds, rare earth tri-tellurides. Near the $M_5$ (3d - 4f) absorption edge of rare earth ions, an intense diffraction peak is detected at a wavevector identical to that of CDW state hosted on Te$_2$ planes, indicating a CDW-induced modulation on the rare earth ions. Surprisingly, the temperature dependence of the diffraction peak intensity demonstrates an exponential increase at low temperatures, vastly different than that of the CDW order parameter. Assuming 4f multiplet splitting due to the CDW states,we pres…
Excitonic insulator (EI) is an intriguing insulating phase of matter, where electrons and holes are bonded into pairs, so called excitons, and form a phase-coherent state via Bose-Einstein Condensation (BEC). Its theoretical concept has been proposed several decades ago, but the followed research is very limited, due to the rare occurrence of EI in natural materials and the lack of manipulating method of excitonic condensation. In this paper, we report the realization of a doping-controlled EI-to-semi-metal transition in Ta$_2$NiSe$_5$ using $in$-$situ$ potassium deposition. Combining with ang…
We report the observation of an extreme magnetoresistance (XMR) in HoBi with a large magnetic moment from Ho f-electrons. Neutron scattering is used to determine the magnetic wave vectors across several metamagnetic (MM) transitions on the phase diagram of HoBi. Unlike other magnetic rare-earth monopnictides, the field dependence of resistivity in HoBi is non-monotonic and reveals clear signatures of every metamagnetic transition in the low-temperature and low-field regime, at T < 2 K and H < 2.3 T. The XMR appears at H > 2.3 T after all the metamagnetic transitions are complete and the system…
Anisotropic metamagnetism and magnetotransport of heavy rare-earth orthorhombic single-crystal TbAlGe
University of Maryland, College Park（马里兰大学帕克分校）；Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室）；National High Magnetic Field Laboratory, Tallahassee（国家高磁场实验室（塔拉哈西））
A number of rare-earth monopnictides have topologically non-trivial band structures together with magnetism and strong electronic correlations. In order to examine whether the antiferromagnetic (AFM) semimetal YbAs ($T\rm_N$ = 0.5 K) exhibits such a scenario, we have grown high-quality single crystals using a flux method, and characterized the magnetic properties and electronic structure using specific heat, magnetotransport and angle-resolved photoemission spectroscopy (ARPES) measurements, together with density functional theory (DFT) calculations. Both ARPES and DFT calculations find no evi…
Existing theoretical works differ on whether three-dimensional Dirac and Weyl semimetals are stable to a short-range-correlated random potential. Numerical evidence suggests the semimetal to be unstable, while some field-theoretic instanton calculations have found it to be stable. The differences go beyond method: the continuum field-theoretic works use a single, perfectly linear Weyl cone, while numerical works use tight-binding lattice models which inherently have band curvature and multiple Weyl cones. In this work, we bridge this gap by performing exact numerics on the same model used in a…
Charge density wave (CDW) states in solids bear an intimate connection to underlying fermiology. Modification of the latter by a suitable perturbation provides an attractive handle to unearth novel CDW states. Here, we combine extensive magnetotransport experiments and first-principles electronic structure calculations on a non-magnetic tritelluride LaTe$_{3}$ single crystal to uncover phenomena rare in CDW systems: $(i)$ hump-like feature in the temperature dependence of resistivity at low temperature under application of magnetic field, which moves to higher temperature with increasing field…
Emergent relativistic quasiparticles in Weyl semimetals are the source of exotic electronic properties such as surface Fermi arcs, the anomalous Hall effect, and negative magnetoresistance, all observed in real materials. Whereas these phenomena highlight the effect of Weyl fermions on the electronic transport properties, less is known about what collective phenomena they may support. Here, we report a new Weyl semimetal, NdAlSi that offers an example. Using neutron diffraction, we report a long-wavelength magnetic order in NdAlSi whose periodicity is linked to the nesting vector between two t…
We have developed and implemented a new ab initio code, CERES (Computational Emulator of Rare Earth Systems), completely written in C++11, which is dedicated to the efficient calculation of the electronic structure and magnetic properties of the crystal field states arising from the splitting of the ground state spin-orbit multiplet in lanthanide complexes. The new code gains efficiency via an optimised implementation of a direct configurational averaged Hartree-Fock (CAHF) algorithm for the determination of $4f$ quasi-atomic active orbitals common to all multi-electron spin manifolds contribu…
