Here, by conducting a systematic $^{89}$Y NMR study, we explore the nature of the magnetic ground state in a newly discovered iron-based superconductor YFe$_2$Ge$_2$. An incoherent-to-coherent crossover due to the Hund's coupling induced electronic correlation is revealed below the crossover temperature $T^*\sim 75\pm15\,\mathrm{K}$. During the electronic crossover, both the Knight shift ($K$) and the bulk magnetic susceptibility ($χ$) exhibit a similar nonmonotonic temperature dependence, and a so-called Knight shift anomaly is also revealed by a careful $K$-$χ$ analysis. Such an electronic crossover has been also observed in heavily hole-doped pnictide superconductors \emph{A}Fe$_2$As$_2$ (\emph{A} = K, Rb, and Cs), which is ascribed to the Hund's coupling induced electronic correlation. Below $T^*$, the spin-lattice relaxation rate divided by temperature $(1/T_1T)$ shows a similar suppression as the Knight shift, suggesting the absence of critical spin fluctuations. This seems to be in conflict with a predicted magnetic quantum critical point (QCP) near this system. However, considering a $\mathbf{q}$-dependent "filter" effect on the transferred hyperfine field, a predominant spin fluctuation with A-type correlation would be perfectly filtered out at $^{89}$Y sites, which is consistent with the recent inelastic neutron scattering results. Therefore, our results confirm that, through a Hund's coupling induced electronic crossover, the magnetic ground state of YFe$_2$Ge$_2$ becomes close to an itinerant magnetic QCP with A-type spin fluctuations. In addition, the possible superconducting pairing due to spin fluctuations is also discussed.
We report x-ray absorption and photoemission spectroscopy of the electronic structure in the normal state of metallic YFe2Ge2. The data reveal evidence for large fluctuating spin moments on the Fe sites, as indicated by exchange multiplets appearing in the Fe 3s core level photoemission spectra, even though the compound does not show magnetic order. The magnitude of the multiplet splitting is comparable to that observed in the normal state of the Fe-pnictide superconductors. This shows a connection between YFe2Ge2 and the Fe-based superconductors even though it contains neither pnictogens nor …
In order to investigate the relationship between the so-called stripe correlations and the high-Tc superconductivity, we have carried out magnetic susceptibility and zero-field muon-spin-relaxation measurements in partially Fe-substituted La2-xSrxCu1-yFeyO4 (LSCFO). It has been found that the Fe substitution induces successive magnetic transitions in the overdoped regime, namely, a spin-glass transition of Fe3+ spins due to the RKKY interaction based on itinerant spins at higher temperatures and a stripe-order transition of localized Cu2+ spins at lower temperatures. The stripe-order transitio…
We study collective spin excitations of a magnetically ordered state in a multi-component system composed of both itinerant electrons and local moments. Here the induced spin-density-wave (SDW) ordering of itinerant electrons and the collinear antiferromangetic (AF) ordering of local moments are locked together via a Hund's rule coupling. We show that the Goldstone theorem still holds at the RPA level with the gapless spin wave protected inside the small SDW gap of itinerant electrons, which, however, is fragile in the presence of ion-anisotropy. A gapped out-of-phase spin mode extending over …
A direct and element-specific measurement of the local Fe spin moment has been provided by analyzing the Fe 3s core level photoemission spectra in the parent and optimally doped CeFeAsO1-xFx (x = 0, 0.11) and Sr(Fe1 xCox)2As2 (x = 0, 0.10) pnictides. The rapid time scales of the photoemission process allowed the detection of large local spin moments fluctuating on a 10-15 s time scale in the paramagnetic, anti-ferromagnetic and superconducting phases, indicative of the occurrence of ubiquitous strong Hund's magnetic correlations. The magnitude of the spin moment is found to vary significantly …
The in-plane resistivity anisotropy has been studied with the Montgomery method on two detwinned parent compounds of the iron-based superconductors, NaFeAs and FeTe. For NaFeAs, the resistivity in the antiferromagnetic (AFM) direction is smaller than that in the ferromagnetic (FM) direction, similar to that observed in BaFe2As2 before. While for FeTe, the resistivity in the AFM direction is larger than that in the FM direction. We show that these two opposite resistivity anisotropy behaviors could be attributed to the strong Hund's rule coupling effects: while the iron pnictides are in the iti…
Different models for doping of two-orbital chains with mobile $S=1/2$ fermions and strong, ferromagnetic (FM) Hund's rule couplings stabilizing the S=1 spins are investigated by density matrix renormalization group (DMRG) methods. The competition between antiferromagnetic (AF) and FM order leads to a rich phase diagram with a narrow FM region for weak AF couplings and strongly enhanced triplet pairing correlations. Without a level difference between the orbitals, the spin gap persists upon doping, whereas gapless spin excitations are generated by interactions among itinerant polarons in the pr…
We characterize the coexistence of itinerant ferromagnetism and spin-triplet superconductivity within a single mechanism involving local (Hund's rule) exchange among $d$ electrons. The ratio of transition temperatures and the spin anisotropy of the superconducting gap is estimated for $ZrZn_2$. The $A$ phase is stable in very low applied and molecular fields, whereas the $A1$ phases persists in higher fields. A small residual magnetic moment is present below the Stoner threshold in the superconducting phase.
We examine the relevance of several major material-dependent parameters to the magnetic softness in iron-base superconductors by first-principles electronic structure analysis of their parent compounds. The results are explained in the spin-fermion model where localized spins and orbitally degenerate itinerant electrons coexist and are coupled by Hund's rule coupling. We found that the difference in the strength of the Hund's rule coupling term is the major material-dependent microscopic parameter for determining the ground-state spin pattern. The magnetic softness in iron-based superconductor…
In most magnetically-ordered iron pnictides, the magnetic moments lie in the FeAs planes, parallel to the modulation direction of the spin stripes. However, recent experiments in hole-doped iron pnictides have observed a reorientation of the magnetic moments from in-plane to out-of-plane. Interestingly, this reorientation is accompanied by a change in the magnetic ground state from a stripe antiferromagnet to a tetragonal non-uniform magnetic configuration. Motivated by these recent observations, here we investigate the origin of the spin anisotropy in iron pnictides using an itinerant microsc…
Superconductivity in bilayer La$_3$Ni$_2$O$_7$: A review focusing on the strong-coupling Hund's rule assisted pairing mechanism
Xiamen University（厦门大学）；Hangzhou Normal University（杭州师范大学）；Beijing Institute of Technology（北京理工大学）；Westlake University（西湖大学）；Westlake Institute for Advanced Study（西湖高等研究院）
We report optical spectroscopic measurements on electron- and hole-doped BaFe2As2. We show that the compounds in the normal state are not simple metals. The optical conductivity spectra contain, in addition to the free carrier response at low frequency, a temperature-dependent gap-like suppression at rather high energy scale near 0.6 eV. This suppression evolves with the As-Fe-As bond angle induced by electron- or hole-doping. Furthermore, the feature becomes much weaker in the Fe-chalcogenide compounds. We elaborate that the feature is caused by the strong Hund's rule coupling effect between …
We report the evolution of nematic fluctuations in FeSe$_{1-x}$S$_x$ single crystals as a function of Sulfur content $x$ across the nematic quantum critical point (QCP) $x_c\sim$ 0.17 via Raman scattering. The Raman spectra in the $B_{1g}$ nematic channel consist of two components, but only the low energy one displays clear fingerprints of critical behavior and is attributed to itinerant carriers. Curie-Weiss analysis of the associated nematic susceptibility indicates a substantial effect of nemato-elastic coupling which shifts the location of the nematic QCP. We argue that this lattice-induce…
We present a two-fluid description for iron-based superconductors, which contains an itinerant electron Fermi-liquid and a local moment spin-liquid, coupled together via an effective Hund's rule interaction. We examine the low-energy collective behavior of such a system. We find that an electron-spinon composite mode emerges in the intermediate coupling regime, which may account for the hump-dip behavior observed in the resent scanning tunneling spectroscopy experiments. The superconductivity and spin-density-wave phases are consistently described within the same framework. Possible experiment…
The alkali-doped fullerides A$_3$C$_{60}$ are half-filled three-orbital Hubbard systems which exhibit an unconventional superconducting phase next to a Mott insulator. While the pairing is understood to arise from an effectively negative Hund coupling, the highly unusual Jahn-Teller metal near the Mott transition, featuring both localized and itinerant electrons, has not been understood. This property is consistently explained by a previously unrecognized phenomenon: the spontaneous transition of multiorbital systems with negative Hund coupling into an orbital-selective Mott state. This symmet…
The varying metallic antiferromagnetic correlations observed in iron-based superconductors are unified in a model consisting of both itinerant electrons and localized spins. The decisive factor is found to be the sensitive competition between the superexchange antiferromagnetism and the orbital-degenerate double-exchange ferromagnetism. Our results reveal the crucial role of Hund's rule coupling for the strongly correlated nature of the system and suggest that the iron-based superconductors are closer kin to manganites than cuprates in terms of their diverse magnetism and incoherent normal-sta…
The importance of the spin-orbit coupling (SOC) effect in Fe-based superconductors (FeSCs) has recently been under hot debate. Considering the Hund's coupling-induced electronic correlation, the understanding of the role of SOC in FeSCs is not trivial and is still elusive. Here, through a comprehensive study of 77Se and 57Fe nuclear magnetic resonance, a nontrivial SOC effect is revealed in the nematic state of FeSe. First, the orbital-dependent spin susceptibility, determined by the anisotropy of the 57Fe Knight shift, indicates a predominant role from the 3dxy orbital, which suggests the coe…
The role of electronic correlations in Condensed Matter is at the heart of various important systems, like magnetic materials, superconductors, topological materials, optical lattices, etc. Electronic correlations are those which change the motion of individual electrons when considering the interaction with other electrons in the material. Among the available systems to study electronic correlation effects, in this thesis I focus on unconventional superconductors, specifically in high-$T_c$ iron-based superconductors, and on two-dimensional materials, like the recent magic-angle twisted bilay…
We show that the combined effects of spin-orbit, monoclinic distortion, and p-d hybridization in tetrahedrally coordinated Fe in LaOFeAs invalidates the naive Hund's rule filling of the Fe d-levels. The two highest occupied levels have one electron each but as a result of the p-d hybridization have very different on-site repulsions. As a result, electrons in the upper level are more itinerant while those in the lower level are more localized. It is the xy-projection of the spin in the lower level that orders antiferromagnetically as the z-components of the spins in the two levels is shown to b…
The magnetic excitations of the iron pnictides are explained within a degenerate double-exchange model. The local-moment spins are coupled by superexchanges $J_1$ and $J_2$ between nearest and next-nearest neighbors, respectively, and interact with the itinerant electrons of the degenerate $d_{xz}$ and $d_{yz}$ orbitals via a ferromagnetic Hund exchange. The latter stabilizes $(π,0)$ stripe antiferromagnetism due to emergent ferro-orbital order and the resulting kinetic energy gain by hopping preferably along the ferromagnetic spin direction. Taking the quantum nature of the spins into account…
Fe-K$_β$ X-ray emission spectroscopy measurements reveal an asymmetric doping dependence of the magnetic moments $μ_\text{bare}$ in electron- and hole-doped BaFe$_{2}$As$_{2}$. At low temperature, $μ_\text{bare}$ is nearly constant in hole-doped samples, whereas it decreases upon electron doping. Increasing temperature substantially enhances $μ_\text{bare}$ in the hole-doped region, which is naturally explained by the theoretically predicted crossover into a spin-frozen state. Our measurements demonstrate the importance of Hund's coupling and electronic correlations, especially for hole-doped …
Hole doping and electronic correlations in Cr-substituted BaFe$_{2}$As$_{2}$
Universidade de São Paulo（圣保罗大学）；European Synchrotron Radiation Facility（欧洲同步辐射装置）；UNICAMP（坎皮纳斯州立大学）；Université de Fribourg（弗里堡大学）；Universidade Federal de Minas Gerais（米纳斯吉拉斯联邦大学）；Ames Laboratory, U.S. DOE（美国能源部艾姆斯实验室）
A d-Electron Heavy-Fermion-Like Superconductor with Frustration-Induced Flat Bands
University of Pittsburgh（匹兹堡大学）；Weizmann Institute of Science（魏茨曼科学研究所）；Ames National Laboratory（艾姆斯国家实验室）；Iowa State University（爱荷华州立大学）；Washington University at St. Louis（圣路易斯华盛顿大学）；University of Arizona（亚利桑那大学）；Oak Ridge National Laboratory（橡树岭国家实验室）；The Pennsylvania State University（宾夕法尼亚州立大学）
In a comprehensive study, we investigate the electronic scattering effects in EuFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ by using Fourier-transform infrared spectroscopy. In spite of the fact that Eu$^{2+}$ local moments order around $T_\text{Eu} \approx 20$\,K, the overall optical response is strikingly similar to the one of the well-known Ba-122 pnictides. The main difference lies within the suppression of the lower spin-density-wave gap feature. By analysing our spectra with a multi-component model, we find that the high-energy feature around 0.7\,eV -- often associated with Hund's rule coupling -…
