Direct measurement of the localized-itinerant transition, hybridization and antiferromagnetic transition of 5f electrons
D. H. Xie, M. L. Li, W. Zhang, L. Huang, W. Feng, Y. Fang, Y. Zhang, Q. Y. Chen, X. G. Zhu, Q. Liu, B. K. Yuan, L. Z. Luo, P. Zhang, X. C. Lai, S. Y. Tan
In heavy-fermion compounds, f electrons show both itinerant and localized behaviour depending on the external conditions, and the hybridization between localized f electrons and itinerant conduction bands gives rise to their exotic properties like heavy-fermions, magnetic orders and unconventional superconductivity. Duo to the risk of handling radioactive actinide materials, the direct experimental evidence of the band structure evolution across the localized-itinerant and magnetic transitions for 5f electrons is lacking. Here, by using angle-resolved photoelectron spectroscopy, we revealed the dual nature (localized vs itinerant) and the development of two different kinds of heavy quasi-particle bands of 5f electrons in antiferromagnetic (AFM) USb2. Partially opened energy gaps were observed on one quasi-particle 5f band cross the AFM transition around 203 K, indicating that the magnetic orders in USb2 are of spin density wave (SDW) type similar to Cr. The localized 5f electrons and itinerant conduction bands hybridize to form another heavy quasi-particle band at about 120 K, and then open hybridization gaps at even lower temperature. Our results provide direct spectral demonstration of the localized-itinerant transition, hybridization and SDW transition of 5f electrons for uranium-based materials.
The discovery of unconventional superconductivity in hole doped NdNiO2, similar to CaCuO2, has received enormous attention. However, different from CaCuO2, RNiO2 (R = Nd, La) has itinerant electrons in the rare-earth spacer layer. Previous studies show that the hybridization between Ni-dx2-y2 and rare-earth-d orbitals is very weak and thus RNiO2 is still a promising analog of CaCuO2. Here, we perform first-principles calculations to show that the hybridization between Ni-dx2-y2 orbital and itinerant electrons in RNiO2 is substantially stronger than previously thought. The dominant hybridizatio…
We investigate the unusual magnetic properties of nearly-critical, weakly-itinerant ferromagnets with general formula UTX, where T=Rh,Co and X=Ge,Si. As a unique feature about these systems, we show that changes in the V_{df} hybridization control their proximity to a ferromagnetic instability, and determine the evolution of: the ground state magnetization, M_0, the Curie Temperature, T_C, the density of states at the Fermi level, N(E_F), the T^2 resistivity coefficient, A, and the specific heat coefficient, γ. The universal aspect of our findings comes from the dependence on only two paramete…
Neutron scattering measurements of the magnetic excitations in single crystals of antiferromagnetic CaFe2As2 reveal steeply dispersive and well-defined spin waves up to an energy of 100 meV. Magnetic excitations above 100 meV and up to the maximum energy of 200 meV are however broader in energy and momentum than the experimental resolution. While the low energy modes can be fit to a Heisenberg model, the total spectrum cannot be described as arising from excitations of a local moment system. Ab-initio calculations of the dynamic magnetic susceptibility suggest that the high energy behavior is …
In a system where selective Mott localization is realized, some electrons show a gap to charge excitations while others do not. A hybridization between these two kind of electrons will lead to a smoothening of this sharp difference and can even bring the system back to a complete delocalization. We show here that there is a large region of parameters at finite hybridization where the selective localization persists and the system shows a partial filling of the selective gap with incoherent states, giving rise to a pseudogap. This result is illustrated here in a two orbital Hubbard model with H…
We report on inelastic neutron scattering measurements that find incommensurate itinerant like magnetic excitations in the normal state of superconducting FeTe$_{0.6}$Se$_{0.4}$ (\Tc=14K) at wave-vector $\mathbf{Q}_{inc}=(1/2\pmε,1/2\mpε)$ with $ε$=0.09(1). In the superconducting state only the lower energy part of the spectrum shows significant changes by the formation of a gap and a magnetic resonance that follows the dispersion of the normal state excitations. We use a four band model to describe the Fermi surface topology of iron-based superconductors with the extended $s(\pm)$ symmetry an…
We use the density matrix renormalization group method to study the interplay of the localized and itinerant behaviors in the one-dimensional Kondo-Heisenberg model. We find signatures of simultaneously localized and itinerant behaviors of the local spins and attribute this duality to their simultaneous entanglement within the spin chain and with conduction electrons due to incomplete hybridization. We propose a microscopic definition of the hybridization parameter that measures this "partial" itinerancy. Our results provide a microscopic support for the dual nature of f-electrons and the resu…
Kondo hybridization in partially filled f-electron systems conveys significant amount of electronic states sharply near the Fermi energy leading to various instabilities from superconductivity to exotic electronic orders. UGe2 is a 5f heavy fermion system, where the Kondo hybridization is interrupted by the formation of two ferromagnetic phases below a 2nd order transition Tc ~ 52 K and a crossover transition Tx ~ 32 K. These two ferromagnetic phases are concomitantly related to a spin-triplet superconductivity that only emerges and persists inside the magnetically ordered phase at high pressu…
We report quantum oscillation measurements that enable the direct observation of the Fermi surface of the low temperature ground state of \ba122. From these measurements we characterize the low energy excitations, revealing that the Fermi surface is reconstructed in the antiferromagnetic state, but leaving itinerant electrons in its wake. The present measurements are consistent with a conventional band folding picture of the antiferromagnetic ground state, placing important limits on the topology and size of the Fermi surface.
A fundamental problem posed from the study of correlated electron compounds, of which heavy-fermion systems are prototypes, is the need to understand the physics of states near a quantum critical point (QCP). At a QCP, magnetic order is suppressed continuously to zero temperature and unconventional superconductivity often appears. Here, we report pressure ($P$) -dependent $^{115}$In nuclear quadrupole resonance (NQR) measurements on heavy-fermion antiferromagnet CeRh$_{0.5}$Ir$_{0.5}$In$_5$. These experiments reveal an antiferromagnetic (AF) QCP at $P_{\rm c}^{\rm AF}$ = 1.2 GPa where a dome o…
We study the competition of Coulomb interaction and hybridization effects in the five-orbital Anderson impurity model by means of continuous time quantum Monte Carlo, exact diagonalization, and Hartree Fock calculations. The dependence of the electronic excitation spectra and thermodynamic ground state properties on hybridization strength and the form of the Coulomb interaction is systematically investigated for impurity occupation number $N \approx 6$. With increasing hybridization strength, a Kondo resonance emerges, broadens and merges with some of the upper and lower Hubbard peaks. Concomi…
This is an analysis of the itinerant model for antiferromagnetism, in which is included both on-site and inter-site electron correlations. We also consider the band degeneration, which brings into the Hamiltonian the on-site exchange interactions. The Green function technique is used and the coherent potential approximation (CPA) decoupling for the on-site Coulomb repulsion. This decoupling combined with the modified Hartree-Fock approximation for the inter-site interactions generates the change in shape of the spin bands with growing interaction constants, which is described by the correlatio…
Cerium (Ce)-based heavy-fermion materials have a characteristic double-peak structure (mid-IR peak) in the optical conductivity [$σ(ω)$] spectra originating from the strong conduction ($c$)--$f$ electron hybridization. To clarify the behavior of the mid-IR peak at a low $c$-$f$ hybridization strength, we compared the $σ(ω)$ spectra of the isostructural antiferromagnetic and heavy-fermion Ce compounds with the calculated unoccupied density of states and the spectra obtained from the impurity Anderson model. With decreasing $c$-$f$ hybridization intensity, the mid-IR peak shifts to the low-energ…
Very often the skyrmions form a triangular crystal in chiral magnets. Here we study the effect of itinerant electrons on the structure of skyrmion crystal (SkX) on triangular lattice using Kondo lattice model in the large coupling limit and treating the localized spins as classical vectors. To simulate the system, we employ hybrid Markov Chain Monte Carlo method (hMCMC) which includes electron diagonalization in each MCMC update for classical spins. We present the low temperature results for $12\times 12$ system at electron density $n=1/3$ which show a sudden jump in skyrmion number when we in…
Neutron diffraction and magnetic susceptibility studies of a polycrystalline SrCr$_2$As$_2$ sample reveal that this compound is an itinerant G-type antiferromagnet below the N${\rm \acute{e}}$el temperature $T_{\textrm N}$ = 590(5) K with the Cr magnetic moments aligned along the tetragonal $c$ axis. The system remains tetragonal to the lowest measured temperature ($\sim$12 K). The lattice parameter ratio $c/a$ and the magnetic moment saturate at about the same temperature below $\sim$ 200 K, indicating a possible magnetoelastic coupling. The ordered moment, $μ=1.9(1)~μ_{\rm B}$/Cr, measured a…
Electrons in solids have been conventionally classified as either band-like itinerant ones or atomic-like localized ones depending on their properties. For heavy Fermion (HF) compounds, however, the f electrons show both itinerant and localized behaviours depending on temperature. Above the characteristic temperature T*, which is typically of the order of few K to few tens K, their magnetic properties are well described by the ionic f-electron models, suggesting that the f-electrons behave as 'localized' electrons. On the other hand, well below T*, their Fermi surfaces (FS's) have been observe…
The generalized decoration-iteration transformation is adopted to treat exactly a hybrid model of doubly decorated two-dimensional lattices, which have localized Ising spins at their nodal lattice sites and itinerant electrons delocalized over pairs of decorating sites. Under the assumption of a half filling of each couple of the decorating sites, the investigated model system exhibits a remarkable spontaneous antiferromagnetic long-range order with an obvious quantum reduction of the staggered magnetization. It is shown that the critical temperature of the spontaneously long-range ordered qua…
By calculating orbitally resolved Pauli susceptibilities within maximally localized Wannier orbital basis transformed from first principles band structures, we find that magnetism in Fe$_{1+x}$Te still has its itinerant origin even without Fermi surface nesting, provided orbital modulation of particle-hole excitations are considered. This leads to strong magnetic instabilities at wave vector (0,$π$)/($π$,0) in d$_{xz}$/d$_{yz}$ orbitals that are responsible for the bicollinear antiferromagnetic state as extra electrons donated from excess Fe are considered. Magnetic exchange coupling between e…
Quantum materials that feature magnetic long-range order often reveal complex phase diagrams when localized electrons become mobile. In many materials magnetism is rapidly suppressed as electronic charges dissolve into the conduction band. In materials where magnetism persists, it is unclear how the magnetic properties are affected. Here we study the evolution of the magnetic structure in Nd(1-x)Ce(x)CoIn(5) from the localized to the highly itinerant limit. We observe two magnetic ground states inside a heavy-fermion phase that are detached from unconventional superconductivity. The presence o…
Using femtosecond time-resolved resonant magnetic x-ray diffraction at the Ho L3 absorption edge, we investigate the demagnetization dynamics in antiferromagnetically ordered metallic Ho after femtosecond optical excitation. Tuning the x-ray energy to the electric dipole (E1, 2p -> 5d) or quadrupole (E2, 2p -> 4f) transition allows us to selectively and independently study the spin dynamics of the itinerant 5d and localized 4f electronic subsystems via the suppression of the magnetic (2 1 3-tau ) satellite peak. We find demagnetization timescales very similar to ferromagnetic 4f systems, sugge…
The interplay of magnetic and superconducting fluctuations in two dimensional systems with van Hove singularities in the electronic spectrum is considered within the functional renormalization group (fRG) approach. While the fRG flow has to be stoped at a certain minimal temperature T_RG^min, we study temperature dependence of magnetic and superconducting susceptibilities both, above and below T_RG^min, which allows to obtain the resulting ground state phase diagram. Close to half filling the fRG approach yields two quantum phase transitions: from commensurate antiferromagnetic to incommensura…
We present the exact solution of a one-dimensional model of a spin-gapped correlated electron system with hybridization impurities exhibiting both magnetic and mixed-valence properties. The host supports superconducting fluctuations, with a spin gap. The localized electrons create a band of antiferromagnetic spin excitations inside the gap for concentrations x of the impurities below some critical value x_c. When x = x_c the spin gap closes and a ferrimagnetic phase appears. This is the first example of an exactly solvable model with coexisting superconducting and antiferromagnetic fluctuation…
Within the framework of density functional theory we investigate the nature of magnetism in various families of Fe-based superconductors. (i) We show that magnetization of stripe-type antiferromagnetic order always becomes stronger when As is substituted by Sb in LaOFeAs, BaFe$_2$As$_2$ and LiFeAs. By calculating Pauli susceptibilities, we attribute the magnetization increase obtained after replacing As by Sb to the enhancement of an instability at $(π,π)$. This points to a strong connection between Fermi surface nesting and magnetism, which supports the theory of the itinerant nature of magne…
In this paper we study an effective model for the normal state of iron-based superconductors. It has separate, but interacting itinerant and localized degrees of freedom, originating from the d_xz and d_yz, and from d_xy iron orbitals respectively. At low temperatures, below a mean-field phase transition, these different states condense together in an excitonic order parameter. We show that at even lower temperature, after another phase transition, this ordered state can spontaneously break the C_4 lattice symmetry and become nematic. We propose this mechanism as an explanation of the tendency…
High-resolution photoemission spectroscopy and realistic ab-initio calculations have been employed to analyze the onset and progression of d-sp hybridization in Fe impurities deposited on alkali metal films. The interplay between delocalization, mediated by the free-electron environment, and Coulomb interaction among d-electrons gives rise to complex electronic configurations. The multiplet structure of a single Fe atom evolves and gradually dissolves into a quasiparticle peak near the Fermi level with increasing the host electron density. The effective multi-orbital impurity problem within th…
In the generic phase diagram of heavy fermion systems, tuning an external parameter such as hydrostatic or chemical pressure modifies the superconducting transition temperature. The superconducting phase forms a dome in the temperature-tuning parameter phase diagram, which is associated with a maximum of the superconducting pairing interaction. Proximity to antiferromagnetism suggests a relation between the disappearance of antiferromagnetic order and superconductivity. We combine muon spin rotation, neutron scattering, and x-ray absorption spectroscopy techniques to gain access to the magneti…
We analyze the metallic (pi,0) antiferromagnetic state of a five-orbital model for iron superconductors. We find that with increasing interactions the system does not evolve trivially from the pure itinerant to the pure localized regime. Instead we find a region with a strong orbital differentiation between xy and yz, which are half-filled gapped states at the Fermi level, and itinerant zx, 3z^2-r^2 and x^2-y^2. We argue that orbital ordering between yz and zx orbitals arises as a consequence of the interplay of the exchange energy in the antiferromagnetic x direction and the kinetic energy ga…
A Kondo-lattice theory is applied to the crossover between local-moment magnetism for almost half fillings of electrons and itinerant-electron magnetism away from the half filling. In clean systems with no disorder, the bandwidth W^* of quasiparticles is non-zero and of the order of |J| at T=0K even in the limit of the half filling, with J the superexchange interaction constant between nearest neighbors. The so called Gutzwiller's term also contributes to W^* away from the half filling; it is approximately proportional to doping concentrations measured from the half filling. Magnetism is enhan…
We report the pressure-dependent optical conductivity spectra of a heavy fermion (HF) compound CeIn3 below the Neel temperature of 10 K to investigate the existence of the HF state in the antiferromagnetic (AFM) phase. The peak due to the interband transition in the hybridization gap between the conduction band and nearly localized 4f states (c-f hybridization) appears at the photon energy of about 20 meV not only in the HF regime but also in the AFM regime. Both the energy and intensity of the c-f hybridization peak continuously increase with the application of pressure from the AFM to the HF…
The electronic structure and magnetism of a new magnetic intercalation compound (Li0.8Fe0.2)OHFeSe are investigated theoretically. The electronic structure calculations predict that the Fe in the (Li,Fe)OH intercalated layer is in +2 valence state, i.e. there is electron doping to the FeSe layer, resulting in the shrinking of the Fermi surface (FS) pocket around Gamma and a strong suppression of dynamical spin susceptibility at M in comparison with the bulk FeSe compound. The ground state of the FeSe layer is a striped antiferromagnetic (SAFM) metal, while the (Li,Fe)OH layer displays a very w…
The CeIn3-xSnx cubic heavy fermion system presents an antiferromagnetic transition at T_N = 10 K, for x = 0, that decreases continuously down to 0 K upon Sn substitution at a critical concentration of x_c ~ 0.65. In the vicinity of T_N -> 0 the system shows non-Fermi liquid behavior due to antiferromagnetic critical fluctuations. For a high Sn content, x > 2.2, intermediate valence effects are present. In this work we show that Gd3+-doped electron spin resonance (ESR) probes a change in the character of the Ce 4f electron, as a function of Sn substitution. The Gd3+ ESR results indicate a trans…
We present a simple, but very realistic, model for a description of pressure induced valence and metal-insulator transitions in mixed valence systems. It is based on the extended Falicov-Kimball model and the supposition that the key interaction governing these transitions is the nonlocal hybridization between the localized $f$ and itinerant $d$ electrons. Taking into account, in addition, the~parametrization between the external pressure and the $d$-$f$ hybridization (the experimental fact), the model is able to describe, at least qualitatively, valence as well as metal-insulator transitions …
We report results of a magnetic and transport study of SrRu1-xMnxO3, i.e., Mn doped SrRuO3. The Mn doping drives the system from the itinerant ferromagnetic state (TC=165 K for x=0) through a quantum critical point at xc=0.39 to an insulating antiferromagnetic state. The onset of antiferromagnetism is abrupt with a Neel temperature increasing from 205 K for x=0.44 to 250 K for x=0.59. Accompanying this quantum phase transition is a drastic change in resistivity by as much as 8 orders of magnitude as a function of x at low temperatures. The critical composition xc=0.39 sharply separates the two…
The electronic structure and magnetism of LiFeO$_{2}$Fe$_{2}$Se$_{2}$ are investigated using the first-principle calculations. The ground state is N$\acute{e}$el antiferromagnetic (AFM) Mott insulating state for Fe1 with localized magnetism in LiFeO$_{2}$ layer and striped AFM metallic state for Fe2 with itinerant magnetism in Fe$_{2}$Se$_{2}$ layer, accompanied with a weak interlayer AFM coupling between Fe1 and Fe2 ions, resulting in a coexistence of localized and itinerant magnetism. Moreover, the layered LiFeO$_{2}$ is found to be more than an insulating block layer but responsible for enh…
We perform quantum Monte Carlo simulations of the itinerant-localized periodic Kondo-Heisenberg model for the underdoped cuprates to calculate the associated spin correlation functions. The strong electron correlations are shown to play a key role in the abrupt destruction of the quasi long-range antiferromagnetic order in the lightly doped regime.
We investigate the spin fluctuations and the pairing symmetry in A$_{x}$Fe$_{2-y}$Se$_{2}$ by the fluctuation exchange approximation. Besides the on-site interactions, the next-nearest-neighbor antiferromagnetic coupling $J_{2}$ is also included. We find that both the itinerant and the localized natures of electrons are important to describe the recent experimental results of the spin fluctuations and the pairing symmetry. In particular, a small $J_{2}$ coupling can change the pairing gap from the d-wave symmetry to the s-wave symmetry. We have also studied the real-space structures of the gap…
We report the discovery of a novel giant magnetoresistance (GMR) phenomenon in a family of BaMn$_{2}$Pn$_{2}$ antiferromagnets (Pn stands for P, As, Sb, and Bi) with a parity-time symmetry. The resistivities of these materials are reduced by $60$ times in magnetic fields ($\vec{H}$'s), thus yielding the GMR of about $-98\%$. The GMR changes systematically along with the Pn elements, hinting that its origin is the spin orbit coupling (SOC) and/or $d$-$p$ orbital hybridization. A positive MR component emerging on top of the negative GMR at low temperatures suggests an orbital-sensitive magnetotr…
The importance of taking into account inter-site $f-f$ hybridization in electron structure calculations for Ce metal and cerium heavy fermion compounds was studied. We demonstrate that for heavy-fermion systems such as cerium compound CeCu$_2$Si$_2$ $f-f$ hybridization can be neglected and Anderson model application is well justified. On another hand for cerium metal $f-f$ hybridization is strong enough to provide the contribution to hybridization function comparable to hybridization between $4f$ and itinerant electrons. We argue that in the case of Ce only the most general Hamiltonian combini…
We report results of 75As nuclear magnetic resonance (NMR) experiments on a self-flux grown single crystal of BaFe2As2. A first-order antiferromagnetic (AF) transition near 135 K was detected by the splitting of NMR lines, which is accompanied by simultaneous structural transition as evidenced by a sudden large change of the electric field gradient tensor at the As site. The NMR results lead almost uniquely to the stripe spin structure in the AF phase. The data of spin-lattice relaxation rate indicate development of anisotropic spin fluctuations of the stripe-type with decreasing temperature i…
We present a detailed temperature and frequency dependence of the optical conductivity measured on clean high quality single crystals of URu$_{2}$Si$_{2}$ of $ac$- and $ab$-plane surfaces. Our data demonstrate the itinerant character of the narrow 5f bands, becoming progressively coherent as temperature is lowered below a cross-over temperature $T^*{\sim}75~K$. $T^*$ is higher than in previous reports as a result of a different sample preparation, which minimizes residual strain. We furthermore present the density-response (energy-loss) function of this compound, and determine the energies of …
Fe3-xGeTe2 is a layered magnetic van der Waals material of interest for both fundamental and applied research. Despite the observation of intriguing physical properties, open questions exist even on the basic features related to magnetism: is it a simple ferromagnet or are there antiferromagnetic regimes and are the moments local or itinerant. Here, we demonstrate that antiferromagnetic spin fluctuations coexist with the ferromagnetism through comprehensive elastic and inelastic neutron scattering and thermodynamic measurements. Our realistic dynamical mean-field theory calculations reveal tha…
We systemically investigate the nature of Ce 4f electrons in structurally layered heavy-fermion compounds CcmMnIn3m+2n (with M =Co, Rh, Ir, and Pt, m=l, 2, n=0 - 2), at low temperature using on-resonance angle-resolved photoemission spectroscopy. Three heavy quasiparticle bands f^0, f^1_7/2 and f^1_5/2 are observed in all compounds, but their intensities and energy locations vary greatly with materials. The strong f^0 states imply that the localized electron behavior dominates the Ce 4f states. The Ce 4f electrons are partially hybridized with the conduction electrons, making them have the dua…
These three metallic systems do not exhibit any magnetic ordering despite experiments show the existence of localized moments with large antiferromagnetic exchange: this is a consequence of the strong geometric frustration (Y(Sc)Mn_{2} and LiV_{2}O_{4} have the Pyrochlore structure, while beta-Mn has a more complicated frustrated structure). Another common feature is their very large specific heat coefficient γ=C/T (420 mJ mole^{-1} K^{-2} for LiV_{2}O_{4}). Several explanations have been proposed for this ''3d heavy fermion behavior'', including a 3d-Kondo effect. However the similarities bet…
Identifying the nature of magnetism, itinerant or localized, remains a major challenge in condensed-matter science. Purely localized moments appear only in magnetic insulators, whereas itinerant moments more or less co-exist with localized moments in metallic compounds such as the doped-cuprate or the iron-based superconductors, hampering a thorough understanding of the role of magnetism in phenomena like superconductivity or magnetoresistance. Here we distinguish two antiferromagnetic modulations with respective propagation wave vectors of $Q_{\pm}$ = ($H \pm 0.557(1)$, 0, $L \pm 0.150(1)$) a…
Based on the {\it ab-initio} band structure for Na$_x$CoO$_2$ we derive the single-electron energies and the effective tight-binding description for the $t_{2g}$ bands using projection procedure. Due to the presence of the next-nearest-neighbor hoppings a local minimum in the electronic dispersion close to the $Γ$ point of the first Brillouin zone forms. Correspondingly, in addition to a large Fermi surface an electron pocket close to the $Γ$ point emerges at high doping concentrations. The latter yields the new scattering channel resulting in a peak structure of the itinerant magnetic suscept…
The Kondo semiconductor CeOs$_{2}$Al$_{10}$ exhibits an antiferromagnetic (AFM) order at $T_\mathrm{N}= 28.5$ K, whose temperature is unexpectedly high for the small ordered moment of $0.3$ $μ_\mathrm{B}/$Ce. We have studied the effects of electron- and hole-doping on the hybridization gap and AFM order by measuring the magnetization $M$, magnetic susceptibility $χ$, electrical resistivity $ρ$, and specific heat $C$ on single crystals of Ce(Os$_{1-x}$Ir$_{x}$)$_{2}$Al$_{10}$($x \le 0.15$) and Ce(Os$_{1-y}$Re$_{y}$)$_{2}$Al$_{10}$($y \le 0.1$). The results of $M (B)$ indicates that the AFM orde…
We address the fundamental question of crossover from localized to itinerant state of a paradigmatic heavy fermionmaterial CeIrIn5. The temperature evolution of the one electron spectra and the optical conductivity is predicted from first principles calculation. The buildup of coherence in the form of a dispersive many body feature is followed in detail and its effects on the conduction electrons and optical conductivity of the material is revealed. We find multiple hybridization gaps and link them to the crystal structure of the material. Our theoretical approach explains the multiple peak st…
Motivated by both experimental and theoretical activities, we discuss the fate of Kondo screening and possible quantum phase transitions in antiferromagnetically ordered phases of Kondo lattices. While transitions with topological changes of the Fermi surface may occur, we demonstrate that an entirely continuous evolution from itinerant to local-moment antiferromagnetism (i.e. from strong to negligible Kondo screening) is possible as well. This situation is in contrast to that in a non-symmetry-broken situation where a quantum phase transition towards an exotic metallic spin-liquid state neces…
Using a hybrid density-functional theory (DFT) calculation including spin-orbit coupling (SOC), we predict that the zigzag antiferromagnetic (AFM) ground state of the honeycomb layered compound Na2IrO3 opens the observed insulating gap through a long-range magnetic order. We show that the effect of SOC and the correction of self-interaction error inherent in previous local or semilocal DFT calculations play crucial roles in predicting the band gap formation in Na2IrO3. It is revealed that the itinerant AFM order with a strong suppression of the Ir magnetic moment is attributed to a considerabl…
Magnetic dc susceptibility ($χ$) and electron spin resonance (ESR) measurements in the paramagnetic regime, are presented. We found a Curie-Weiss (CW) behavior for $χ$(T) with a ferromagnetic $Θ= 446(5)$ K and $μ_{eff} = 4.72(9) μ_{B}/f.u.$, this being lower than that expected for either $Fe^{3+}(5.9μ_{B})$ or $Fe^{2+}(4.9μ_{B})$ ions. The ESR g-factor $g = 2.01(2)$, is associated with $Fe^{3+}$. We obtained an excellent description of the experiments in terms of two interacting sublattices: the localized $Fe^{3+}$ ($3d^{5}$) cores and the delocalized electrons. The coupled equations were solv…
We present the ultralow-temperature specific heat and thermal conductivity measurements on single crystals of triangular-lattice antiferromagnet Na$_2$BaCo(PO$_4$)$_2$, which was recently argued to host itinerant fermionic excitations, like a quantum spin liquid, above its antiferromagnetic phase transition temperature $T_{\rm N}$ = 0.148 K. In specific heat measurements, we confirm the peaks due to antiferromagnetic ordering when magnetic field $μ_0 H \leq$ 1 T, roughly consistent with previous work [N. Li $et$ $al.$, Nat. Commun. 11, 4216 (2020)]. However, in thermal conductivity measurement…
The weak antiferromagnetism of URu${}_{2}$Si${}_{2}$ is discussed on the basis of a duality model which takes into account salient features of both itinerant fermions and "localized" component of spin degrees of freedom. The problem is analyzed in the framework of induced-moment mechanism by taking a singlet-singlet crystal field scheme together with the nesting property of partial Fermi surface of itinerant fermions . It is shown that the extremely small ordered moment $m$ of ${\cal O}$($10^{-2}$$\times$$μ_{B}$) can be compatible with the large specific-heat jump at the transition temperature…
Metallic quantum criticality is among the central theme in the understanding of correlated electronic systems, and converging results between analytical and numerical approaches are still under calling. In this work, we develop state-of-art large scale quantum Monte Carlo simulation technique and systematically investigate the itinerant quantum critical point on a 2D square lattice with antiferromagnetic spin fluctuations at wavevector $\mathbf{Q}=(π,π)$ -- a problem that resembles the Fermi surface setup and low-energy antiferromagnetic fluctuations in high-Tc cuprates and other critical meta…
A phenomenological model with itinerant bands and local states trapped by the lattice on the Cu-sites, is discussed to describe global features of cuprates. Relative energy positions of localized and itinerant states being tuned (thermodynamically or by doping), the system must undergo 1st order Mott metal-insulator transition. Decreasing the local level (from the metallic end of a stoichiometric compound), charge separation instability occurs first before the Mott transition. Crossing and hybridization between local (flat) and itinerant bands introduce a structure in density of states which m…
The temperature-dependent evolution pattern of 5f electrons helps to elucidate the long-standing itinerant-localized dual nature in plutonium-based compounds. In this work, we investigate the correlated electronic states of PuIn3 dependence on temperature by using a combination of the density functional theory and the dynamical mean-field theory. Not only the experimental photoemission spectroscopy is correctly reproduced, but also a possible hidden 5f itinerant-localized crossover is identified. Moreover, it is found that the quasiparticle multiplets from the many-body transitions gradually e…
