Evidence for large thermodynamic signatures of in-gap fermionic quasiparticle states in a Kondo insulator.

The mixed-valence compound YbB12 displays paradoxical quantum oscillations in electrical resistivity and magnetic torque in a regime with a well-developed insulating charge gap and in the absence of an electronic Fermi surface. However, signatures of such unusual fermionic quasiparticles in other bulk thermodynamic observables have been missing. Here we report the observation of a series of sharp double-peak features in the specific heat as a function of the magnetic field. The measured Hall resistivity evolves smoothly across the field values at which the characteristic anomalies appear in the thermodynamic response and rules out the possibility of conventional electrons as their origin. Our observations of thermodynamic anomalies in a bulk three-dimensional electrical insulator provide the evidence for the presence of emergent dispersing fermionic excitations within the insulating bulk, which sets the stage for further investigation of electron fractionalization in other correlated mixed-valence compounds.

Detecting Magnetoelectric Effect in a Metallic Antiferromagnet via Nonreciprocal Rotation of Reflected Light.

Certain types of media breaking both space-inversion (P) and time-reversal (T) symmetries but preserving their combination PT exhibit the polarization rotation of reflected light even when that of transmitted light is prohibited. Such an effect is termed nonreciprocal rotation of reflected light (NRR). Although NRR shows nearly the same phenomenon as the magnetooptical Kerr effect or, equivalently, the Hall effect at optical frequencies, its origin is distinct and ascribed to a magnetoelectric (ME) effect at optical frequencies, i.e., the optical ME effect. Here we show the observation of NRR in a metallic antiferromagnet TbB_{4}. The result demonstrates that the ME effect in a metallic system, which is considered to be ill defined, can be detected using reflected light. Furthermore, we spatially resolve antiferromagnetic domains in TbB_{4} by microscope observations of NRR. Our work offers a unique way to probe the ME effect in metallic systems.

Breakdown of bulk-projected isotropy in surface electronic states of topological Kondo insulator SmB6(001).

The topology and spin-orbital polarization of two-dimensional (2D) surface electronic states have been extensively studied in this decade. One major interest in them is their close relationship with the parities of the bulk (3D) electronic states. In this context, the surface is often regarded as a simple truncation of the bulk crystal. Here we show breakdown of the bulk-related in-plane rotation symmetry in the topological surface states (TSSs) of the Kondo insulator SmB6. Angle-resolved photoelectron spectroscopy (ARPES) performed on the vicinal SmB6(001)-p(2 × 2) surface showed that TSSs are anisotropic and that the Fermi contour lacks the fourfold rotation symmetry maintained in the bulk. This result emphasizes the important role of the surface atomic structure even in TSSs. Moreover, it suggests that the engineering of surface atomic structure could provide a new pathway to tailor various properties among TSSs, such as anisotropic surface conductivity, nesting of surface Fermi contours, or the number and position of van Hove singularities in 2D reciprocal space.

High-Pressure Synthesis of Light Lanthanide Dodecaborides (PrB12 and CeB12): Effects of Valence Fluctuation on Volume and Formation Pressure.

Light lanthanide dodecaborides, RB12 (R = Pr and Ce), were synthesized from a stoichiometric mixture of hexaborides and boron using a laser-heated diamond anvil cell under high-pressure and high-temperature conditions. Contrary to the expectation that lighter lanthanide elements require higher pressure to crystallize RB12, in situ X-ray diffraction experiments reveal that cerium dodecaboride crystallizes at 26 GPa, which is significantly lower than that required to form the heavier praseodymium dodecaboride (35 GPa). In addition to the lower formation pressure, an anomalous volume reduction is also observed in CeB12, which can be explained by a valence fluctuation between Ce3+ and Ce4+ indicated by X-ray absorption near-edge structure measurements. A polyhedral coordination change from a truncated cube in RB6 to a truncated octahedron in RB12 and associated shortening of the R-B bond length result in an increase in bulk modulus and hardness.

Non-trivial surface states of samarium hexaboride at the (111) surface.

The peculiar metallic electronic states observed in the Kondo insulator, samarium hexaboride (SmB6), has stimulated considerable attention among those studying non-trivial electronic phenomena. However, experimental studies of these states have led to controversial conclusions mainly due to the difficulty and inhomogeneity of the SmB6 crystal surface. Here, we show the detailed electronic structure of SmB6 with angle-resolved photoelectron spectroscopy measurements of the three-fold (111) surface where only two inequivalent time-reversal-invariant momenta (TRIM) exist. We observe the metallic two-dimensional state was dispersed across the bulk Kondo gap. Its helical in-plane spin polarisation around the surface TRIM indicates that SmB6 is topologically non-trivial, according to the topological classification theory for weakly correlated systems. Based on these results, we propose a simple picture of the controversial topological classification of SmB6.

Magnetic-Field-Induced Kondo Metal Realized in YbB_{12}.

The specific heat of the Kondo insulator YbB_{12} has been measured up to 60 T. The Sommerfeld coefficient γ significantly increases at around 50 T, where the insulator metal transition occurs with a steep increase of the magnetization. γ reaches 67 mJ/(mol K^{2}) at high fields, which directly indicates that the quasiparticles gain a heavy thermodynamic effective mass and transform into a Kondo metal under magnetic fields. The field-induced Kondo metal has a rather high Kondo temperature around 200 K. The strong Kondo coupling proves that the energy gap collapse does not correspond to the breakdown of the Kondo bound state. The steep increase of the magnetization at the transition manifests the sharp density of states at the Fermi energy formed via the Kondo resonance.

Evidence for in-gap surface states on the single phase SmB6(001) surface.

Structural and electronic properties of the SmB6(001) single-crystal surface prepared by Ar+ ion sputtering and controlled annealing are investigated by scanning tunneling microscopy. In contrast to the cases of cleaved surfaces, we observe a single phase surface with a non-reconstructed p(1 × 1) lattice on the entire surface at an optimized annealing temperature. The surface is identified as Sm-terminated on the basis of spectroscopic measurements. On a structurally uniform surface, the emergence of the in-gap state, a robust surface state against structural variation, is further confirmed inside a Kondo hybridization gap at 4.4 K by temperature and atomically-resolved spatial dependences of the differential conductance spectrum near the Fermi energy.

Surface Kondo effect and non-trivial metallic state of the Kondo insulator YbB12.

A synergistic effect between strong electron correlation and spin-orbit interaction has been theoretically predicted to realize new topological states of quantum matter on Kondo insulators (KIs), so-called topological Kondo insulators (TKIs). One TKI candidate has been experimentally observed on the KI SmB6(001), and the origin of the surface states (SS) and the topological order of SmB6 has been actively discussed. Here, we show a metallic SS on the clean surface of another TKI candidate YbB12(001) using angle-resolved photoelectron spectroscopy. The SS shows temperature-dependent reconstruction corresponding to the Kondo effect observed for bulk states. Despite the low-temperature insulating bulk, the reconstructed SS with c-f hybridization is metallic, forming a closed Fermi contour surrounding on the surface Brillouin zone and agreeing with the theoretically expected behaviour for SS on TKIs. These results demonstrate the temperature-dependent holistic reconstruction of two-dimensional states localized on KIs surface driven by the Kondo effect.

X-ray atomic orbital analysis of 4f and 5d electron configuration of SmB6 at 100, 165, 230 and 298 K.

Accurate electron-density measurement of SmB(6) at 100, 165, 230 and 298 K, and X-ray atomic orbital (XAO) analysis were carried out. The 4f-electron density around Sm and 5d electron density at approximately 1 A from Sm were analysed by XAO analysis. The 5d electron density is due to the electrons of the 5d(J = 5/2)Gamma(8) orbitals which stem from the e(g) orbitals in the strong field approximation. The change in electron populations of the 5d(5/2)Gamma(8) orbitals with temperature is similar to that of the resistivity. Since the conduction band consists of 5d(5/2)Gamma(8) and B-2p orbitals according to band theory, this indicates that the larger populations of the 5d(5/2)Gamma(8) orbitals correspond to the larger number of localized electrons and are correlated to the resistivity of SmB(6). The occupation of the bulky 5d(5/2)Gamma(8) orbitals may be the reason for the elongation of the lattice parameter below 150 K. The 4f(7/2)Gamma(6) orbitals are obviously occupied except at 100 K, which seems to be caused by the energy gap between 4f(5/2) and 4f(7/2) states, which begins to exist between 100 and 150 K, and may represent one of the properties of a Kondo insulator.

Magnetic field induced 4f octupole in CeB6 probed by resonant x-ray diffraction.

A mysterious antiferroquadrupolar ordered phase of CeB6 is considered as originating from the Txyz-type magnetic octupole moment in magnetic fields. By resonant x-ray diffraction, we have verified that the Txyz-type octupole is indeed induced in the 4f orbital of Ce with a propagation vector (1/2,1/2,1/2), thereby supporting the theory. We observed an asymmetric field dependence of the intensity for an electric quadrupole (E2) resonance when the field was reversed and extracted a field dependence of the octupole by utilizing the interference with an electric dipole (E1) resonance. The result is in good agreement with that of the NMR-line splitting, which reflects the transferred hyperfine field at the boron nucleus from the anisotropic spin distribution of Ce with an Oxy-type quadrupole.