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Electrons in localized 4f orbitals around lanthanide elements in solids are dominated by strong spin-orbit coupling. The resultant J multiplets are further split by the crystalline electric field, where J denotes the total angular momentum quantum number, and hence exhibit anisotropic spatial distribution. The anisotropy of spin-orbit entangled 4f electrons is closely linked to their physical properties. Here, we demonstrate the visualization of 4f electrons in pyrochlore oxides A2Ir2O7 (A = Pr, Nd, and Eu) by combining high-photon-energy X-ray diffraction and valence electron density (VED) analysis based on the core differential Fourier synthesis (CDFS) method. The observed VED distributions around the A site roughly agree with point-charge calculations, considering the relativistic spin-orbit coupling and the trigonal crystal electric field under the LS coupling scheme. The CDFS-based VED observation method can be applied to the analysis of the 4f state of various crystalline materials., Comment: 19 pages, 3 figures, SI

When a conduction electron couples with a non-coplanar localized magnetic moment, the realspace Berry curvature is exerted to cause the geometrical Hall effect, which is not simply proportional to the magnetization. So far, it has been identified in the case mostly where the non-coplanar magnetic order is present on the sublattice of conduction electrons. Here, we demonstrate that the geometrical Hall effect shows up even without long-range magnetic order of conduction electrons, as induced by non-coplanar exchange fields from the localized magnetic moments, in hole-doped phyrochlore molybdates. We find that the geometrical Hall effect is markedly anisotropic with respect to the applied magnetic field direction, which is in good accordance with the field-dependent magnitude and sign change of the real-space scalar spin chirality of local Tb moments. These results may facilitate the understanding of emergent electromagnetic responses induced by the Kondo-like coupling between conduction electrons and local spins in a broad material class., Comment: 9 pages, 7 figures

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 in the momentum space strongly depends on the respective electronic state as well as on the Kondo coupling strength. These observations pave a route toward the engineering of band topology in hybrid quantum materials with relativistic conduction electrons and localized magnetic moments.

The quest for nonmagnetic Weyl semimetals with high tunability of phase has remained a demanding challenge. As the symmetry breaking control parameter, the ferroelectric order can be steered to turn on/off the Weyl semimetals phase, adjust the band structures around the Fermi level, and enlarge/shrink the momentum separation of Weyl nodes which generate the Berry curvature as the emergent magnetic field. Here, we report the realization of a ferroelectric nonmagnetic Weyl semimetal based on indium doped Pb1 xSnxTe alloy where the underlying inversion symmetry as well as mirror symmetry is broken with the strength of ferroelectricity adjustable via tuning indium doping level and Sn/Pb ratio. The transverse thermoelectric effect, i.e., Nernst effect both for out of plane and in plane magnetic field geometry, is exploited as a Berry curvature sensitive experimental probe to manifest the generation of Berry curvature via the redistribution of Weyl nodes under magnetic fields. The results demonstrate a clean non-magnetic Weyl semimetal coupled with highly tunable ferroelectric order, providing an ideal platform for manipulating the Weyl fermions in nonmagnetic system., Comment: 20 pages, 4 figures

Carrier doping to the Mott insulator is essential to produce highly correlated metals with emergent properties. Pyrochlore ruthenates, Pr$_{2}$Ru$_{2}$O$_{7}$ (Ru-$4d$ electron number, $n=4$) and Ca$_{2}$Ru$_{2}$O$_{7}$ ($n=3$), are a Mott insulator and a magnetic bad metal, respectively, due to the strong electron correlation. We investigate magneto-transport properties of (Pr$_{1-x}$Ca$_{x}$)$_{2}$Ru$_{2}$O$_{7}$ in a whole band-filling range, $0

We study possible Weyl semimetals of strongly-correlated electrons by investigating magnetotransport properties in pyrochlore R2Ir2O7 (R=rare-earth ions), choosing three types of R ions to design the exchange coupling scheme between R 4f and Ir 5d moments; non-magnetic Eu (4f6), isotropic Gd (4f7), and anisotropic Tb (4f8). In the doping-induced semimetallic state, distinctive features of magnetoresistance and Hall effect are observed in R=Gd and Tb compounds due to the effects of the exchange-enhanced isotropic and anisotropic Zeeman fields, respectively, exemplifying the double Weyl semimetal and the 2-in 2-out line-node semimetal as predicted by theories. In particular, a Hall angle of R=Gd compound is strongly enhanced to 1.5 % near above the critical doping for the Mott transition. Furthermore, an unconventional Hall contribution is discerned for a lower doping regime of R=Gd compound, which can be ascribed to the emergence of Weyl points with the field-distorted all-in all-out order state. These findings indicate that the hole-doping induced Mott transition as well as the characteristic f-d exchange interaction stabilizes versatile topological semimetal states in a wide range of material parameter space., Comment: 8 pages, 10 figures

In the context of correlated insulators, where electron-electron interactions (U) drive the localization of charge carriers, the metal-insulator transition (MIT) is described as either bandwidth (BC) or filling (FC) controlled. Motivated by the challenge of the insulating phase in Sr$_2$IrO$_4$, a new class of correlated insulators has been proposed, in which spin-orbit coupling (SOC) is believed to renormalize the bandwidth of the half-filled $j_{\mathrm{eff}} = 1/2$ doublet, allowing a modest U to induce a charge-localized phase. Although this framework has been tacitly assumed, a thorough characterization of the ground state has been elusive. Furthermore, direct evidence for the role of SOC in stabilizing the insulating state has not been established, since previous attempts at revealing the role of SOC have been hindered by concurrently occurring changes to the filling. We overcome this challenge by employing multiple substituents that introduce well defined changes to the signatures of SOC and carrier concentration in the electronic structure, as well as a new methodology that allows us to monitor SOC directly. Specifically, we study Sr$_2$Ir$_{1-x}$T$_x$O$_4$ (T = Ru, Rh) by angle-resolved photoemission spectroscopy (ARPES), combined with ab-initio and supercell tight-binding calculations. This allows us to distinguish relativistic and filling effects, thereby establishing conclusively the central role of SOC in stabilizing the insulating state of Sr$_2$IrO$_4$. Most importantly, we estimate the critical value for spin-orbit coupling in this system to be $\lambda_c = 0.42 \pm 0.01$ eV, and provide the first demonstration of a spin-orbit-controlled MIT.