Rare-earth intermetallic compounds exhibit rich phenomena induced by the interplay between localized f orbitals and conduction electrons. However, since the energy scale of the crystal-electric-field splitting is only a few millielectronvolts, the nature of the mobile electrons accompanied by collective crystal-electric-field excitations has not been unveiled. Here, we examine the low-energy electronic structures of CeSb through the anomalous magnetostructural transitions below the Néel temperature, ~17 K, termed the ‘devil’s staircase’, using laser angle-resolved photoemission, Raman and neutron scattering spectroscopies. We report another type of electron–boson coupling between mobile electrons and quadrupole crystal-electric-field excitations of the 4 f orbitals, which renormalizes the Sb 5 p band prominently, yielding a kink at a very low energy (~7 meV). This coupling strength is strong and exhibits anomalous step-like enhancement during the devil’s staircase transition, unveiling a new type of quasiparticle, named the ‘multipole polaron’, comprising a mobile electron dressed with a cloud of the quadrupole crystal-electric-field polarization.
Nematicity is ubiquitous in the electronic phases of iron-based superconductors. The order parameter that characterizes the nematic phase has been investigated in momentum space, but its real-space arrangement remains largely unexplored. We use linear dichroism (LD) in a low-temperature laser–photoemission electron microscope to map out the nematic order parameter of nonmagentic FeSe and antiferromagnetic BaFe2(As0.87P0.13)2. In contrast to structural domains, which have atomic-scale domain walls, the LD patterns in both materials show peculiar sinusoidal waves of electronic nematicity with wavelengths more than 1000 times as long as the unit cell. Our findings put strong constraints on the theoretical investigation of electronic nematicity.
Y. Arai, Kenta Kuroda, T. Nomoto, Z. H. Tin, S. Sakuragi, C. Bareille, S. Akebi, K. Kurokawa, Y. Kinoshita, W.-L. Zhang, 4 S. Shin, M. Tokunaga, H. Kitazawa, Y. Haga, H. S. Suzuki, S. Miyasaka, S. Tajima, K. Iwasa, R. Arita, 8 and Takeshi Kondo 9 ISSP, University of Tokyo, Kashiwa, Chiba 277-8581, Japan Department of Applied Physics, University of Tokyo, 7-3-1 Hongo Bunkyo-ku, Tokyo 113-8656, Japan Department of Physics, Osaka University, Osaka 560-0043, Japan Department of Engineering and Applied Sciences, Sophia University, 7-1 Kioicho, Chiyoda-ku, Tokyo, 102-8554, Japan National Institute for Materials Science, 1-2-1 Sengen, Tsukuba 305-0047, Japan Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195, Japan Frontier Research Center for Applied Atomic Sciences and Institute of Quantum Beam Science, Ibaraki University, Tokai, Naka, Ibaraki 319-1106, Japan RIKEN Center for Emergent Matter Science (CEMS), 2-1 Hirosawa, Wako, Saitama 351-0198, Japan Trans-scale Quantum Science Institute, University of Tokyo, Bunkyo-ku, Tokyo 113-0033, Japan
Multi-layered materials provide fascinating platforms to realize various functional properties, possibly leading to future electronic devices controlled by external fields. In particular, layered magnets coupled with conducting layers have been extensively studied recently for possible control of their transport properties via the spin structure. Successful control of quantum-transport properties in the materials with antiferromagnetic (AFM) layers, so-called natural spin-valve structure, has been reported for the Dirac Fermion and topological/axion materials. However, a bulk crystal in which magnetic and superconducting layers are alternately stacked has not been realized until now, and the search for functional properties in it is an interesting yet unexplored field in material science. Here, we discover superconductivity providing such an ideal platform in EuSn2As2 with the van der Waals stacking of magnetic Eu layers and superconducting Sn-As layers, and present the first demonstration of a natural spin-valve effect on the superconducting current. Below the superconducting transition temperature (Tc), the electrical resistivity becomes zero in the in-plane direction. In contrast, it, surprisingly, remains finite down to the lowest temperature in the out-of-plane direction, mostly due to the structure of intrinsic magnetic Josephson junctions in EuSn2As2. The magnetic order of the Eu layers (or natural spin-valve) is observed to be extremely soft, allowing one to easy control of the out-of-plane to in-plane resistivities ratio from 1 to infinity by weak external magnetic fields. The concept of multi-functional materials with stacked magnetic-superconducting layers will open a new pathway to develop novel spintronic devices with magnetically controllable superconductivity.
Interfacing bulk conducting topological Bi_{2}Se_{3} films with s-wave superconductors initiates strong superconducting order in the nontrivial surface states. However, bulk insulating topological (Bi_{1-x}Sb_{x})_{2}Te_{3} films on bulk Nb instead exhibit a giant attenuation of surface superconductivity, even for films only two layers thick. This massive suppression of proximity pairing is evidenced by ultrahigh-resolution band mappings and by contrasting quantified superconducting gaps with those of heavily n-doped topological Bi_{2}Se_{3}/Nb. The results underscore the limitations of using superconducting proximity effects to realize topological superconductivity in nearly intrinsic systems.
Solids with competing interactions often undergo complex phase transitions with a variety of long-periodic modulations. Among such transition, devil’s staircase is the most complex phenomenon, and for it, CeSb is the most famous material, where a number of the distinct phases with long-periodic magnetostructures sequentially appear below the Néel temperature. An evolution of the low-energy electronic structure going through the devil’s staircase is of special interest, which has, however, been elusive so far despite 40 years of intense research. Here, we use bulk-sensitive angle-resolved photoemission spectroscopy and reveal the devil’s staircase transition of the electronic structures. The magnetic reconstruction dramatically alters the band dispersions at each transition. Moreover, we find that the well-defined band picture largely collapses around the Fermi energy under the long-periodic modulation of the transitional phase, while it recovers at the transition into the lowest-temperature ground state. Our data provide the first direct evidence for a significant reorganization of the electronic structures and spectral functions occurring during the devil’s staircase.
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Experimental determinations of bulk band topology in the solid states have been so far restricted to only indirect investigation through the probing of surface states predicted by electronic structure calculations. We here present an alternative approach to determine the band topology by means of bulk-sensitive soft x-ray angle-resolved photoemission spectroscopy. We investigate the bulk electronic structures of the series materials, Ce monopnictides (CeP, CeAs, CeSb, and CeBi). By performing a paradigmatic study of the band structures as a function of their spin-orbit coupling, we draw the topological phase diagram and unambiguously reveal the topological phase transition from a trivial to a nontrivial regime in going from CeP to CeBi induced by the band inversion. The underlying mechanism of the phase transition is elucidated in terms of spin-orbit coupling in concert with their semimetallic band structures. Our comprehensive observations provide a new insight into the band topology hidden in the bulk states.
We reveal the orbital-selective metal-insulator transition in a 4d multiorbital system, Sr-3(Ru1-xMnx)(2)O-7 (x = 0-0.2), by means of angle-resolved photoemission spectroscopy. With a small substitution (x = 0.05) of Mn with localized 3d orbitals, the spectra for the 4d(xy) band become incoherent with a large gap, while the 4d(xz/yz) bands stay metallic with sharp quasiparticle peaks. Intriguingly, this lifts band hybridization among 4d orbitals, and causes a two-to one-dimensional crossover in the remaining Fermi surface. Significant nesting in the remaining Fermi surface is implied to induce the reported magnetic ordering, and yields the insulating bulk state at higher Mn substitution, where all bands are gapped and totally incoherent. The availability of orbital-selective tuning of the pseudogap by a small impurity will prompt further theoretical studies of Hund's metals, which were recognized only recently in condensed matter physics.
We reveal the orbital-selective metal-insulator transition in a $4d$ multiorbital system, ${\mathrm{Sr}}_{3}{({\mathrm{Ru}}_{1\ensuremath{-}x}{\mathrm{Mn}}_{x})}_{2}{\mathrm{O}}_{7}\phantom{\rule{4pt}{0ex}}(x=0\ensuremath{-}0.2)$, by means of angle-resolved photoemission spectroscopy. With a small substitution $(x=0.05)$ of Mn with localized $3d$ orbitals, the spectra for the $4{d}_{xy}$ band become incoherent with a large gap, while the $4{d}_{xz/yz}$ bands stay metallic with sharp quasiparticle peaks. Intriguingly, this lifts band hybridization among $4d$ orbitals, and causes a two- to one-dimensional crossover in the remaining Fermi surface. Significant nesting in the remaining Fermi surface is implied to induce the reported magnetic ordering, and yields the insulating bulk state at higher Mn substitution, where all bands are gapped and totally incoherent. The availability of orbital-selective tuning of the pseudogap by a small impurity will prompt further theoretical studies of Hund's metals, which were recognized only recently in condensed matter physics.
R. Noguchi, T. Takahashi, K. Kuroda, M. Ochi, T. Shirasawa, M. Sakano, 5 C. Bareille, M. Nakayama, M. D. Watson, K. Yaji, A. Harasawa, H. Iwasawa, P. Dudin, T. K. Kim, M. Hoesch, S. Shin, R. Arita, T. Sasagawa, and Takeshi Kondo* Institute for Solid State Physics, University of Tokyo, Kashiwa, Chiba 277-8581, Japan Materials and Structures Laboratory, Tokyo Institute of Technology, Yokohama, Kanagawa 226-8503, Japan Department of Physics, Osaka University, Toyonaka, Osaka 560-0043, Japan National Metrology Institute of Japan, National Institute of Advanced Industrial Science and Technology, Tsukuba, Ibaraki 305-8565, Japan Department of Applied Physics and Quantum-Phase Electronics Center (QPEC), The University of Tokyo, Tokyo 113-8656, Japan Diamond Light Source, Harwell Campus, Didcot, OX11 0DE, United Kingdom RIKEN Center for Emergent Matter Science (CEMS), Wako, Saitama 351-0198, Japan (Dated: February 9, 2018)
Experimental evidence for the realization of magnetic Weyl fermions in the strongly correlated metal Mn3Sn is reported. Weyl fermions1,2,3 have been observed as three-dimensional, gapless topological excitations in weakly correlated, inversion-symmetry-breaking semimetals4,5. However, their realization in spontaneously time-reversal-symmetry-breaking phases of strongly correlated materials has so far remained hypothetical2,6,7. Here, we report experimental evidence for magnetic Weyl fermions in Mn3Sn, a non-collinear antiferromagnet that exhibits a large anomalous Hall effect, even at room temperature8. Detailed comparison between angle-resolved photoemission spectroscopy (ARPES) measurements and density functional theory (DFT) calculations reveals significant bandwidth renormalization and damping effects due to the strong correlation among Mn 3d electrons. Magnetotransport measurements provide strong evidence for the chiral anomaly of Weyl fermions—namely, the emergence of positive magnetoconductance only in the presence of parallel electric and magnetic fields. Since weak magnetic fields (approximately 10 mT) are adequate to control the distribution of Weyl points and the large fictitious fields (equivalent to approximately a few hundred T) produced by them in momentum space, our discovery lays the foundation for a new field of science and technology involving the magnetic Weyl excitations of strongly correlated electron systems such as Mn3Sn.
We present an angle-resolved photoemission study of the electronic structure of the three-dimensional pyrochlore iridate Nd_{2}Ir_{2}O_{7} through its magnetic metal-insulator transition. Our data reveal that metallic Nd_{2}Ir_{2}O_{7} has a quadratic band, touching the Fermi level at the Γ point, similar to that of Pr_{2}Ir_{2}O_{7}. The Fermi node state is, therefore, a common feature of the metallic phase of the pyrochlore iridates. Upon cooling below the transition temperature, this compound exhibits a gap opening with an energy shift of quasiparticle peaks like a band gap insulator. The quasiparticle peaks are strongly suppressed, however, with further decrease of temperature, and eventually vanish at the lowest temperature, leaving a nondispersive flat band lacking long-lived electrons. We thereby identify a remarkable crossover from Slater to Mott insulators with decreasing temperature. These observations explain the puzzling absence of Weyl points in this material, despite its proximity to the zero temperature metal-insulator transition.
We report the existence of confined electronic states at the (110) and (111) surfaces of SrTiO3. Using angle-resolved photoemission spectroscopy, we find that the corresponding Fermi surfaces, subband masses, and orbital ordering are different from the ones at the (001) surface of SrTiO3. This occurs because the crystallographic symmetries of the surface and sub-surface planes, and the electron effective masses along the confinement direction, influence the symmetry of the electronic structure and the orbital ordering of the t2g manifold. Remarkably, our analysis of the data also reveals that the carrier concentration and thickness are similar for all three surface orientations, despite their different polarities. The orientational tuning of the microscopic properties of two-dimensional electron states at the surface of SrTiO3 echoes the tailoring of macroscopic (e.g. transport) properties reported recently in LaAlO3/SrTiO3 (110) and (111) interfaces, and is promising for searching new types of 2D electronic states in correlated-electron oxides.
Two-dimensional electron gases (2DEGs) at transition-metal oxide (TMO) interfaces and boundary states in topological insulators, are being intensively investigated. The former system harbors superconductivity, large magneto-resistance and ferromagnetism. In the latter, honeycomb-lattice geometry plus bulk spin-orbit interactions lead to topologically protected spin-polarized bands. 2DEGs in TMOs with a honeycomb-like structure could yield new states of matter, but they had not been experimentally realized, yet. We successfully created a 2DEG at the (111) surface of KTaO3, a strong insulator with large spin-orbit coupling. Its confined states form a network of weakly-dispersing electronic gutters with 6-fold symmetry, a topology novel to all known oxide-based 2DEGs. If those pertain to just one Ta-(111) bilayer, model calculations predict that it can be a topological metal. Our findings demonstrate that completely new electronic states, with symmetries not realized in the bulk, can be tailored in oxide surfaces, promising for TMO-based devices.
Spontaneous symmetry breaking in physical systems leads to salient phenomena at all scales, from the Higgs mechanism and the emergence of the mass of the elementary particles, to superconductivity and magnetism in solids. The hidden-order state arising below 17.5 K in URu2Si2 is a puzzling example of one of such phase transitions: its associated broken symmetry and gap structure have remained longstanding riddles. Here we directly image how, across the hidden-order transition, the electronic structure of URu2Si2 abruptly reconstructs. We observe an energy gap of 7 meV opening over 70% of a large diamond-like heavy-fermion Fermi surface, resulting in the formation of four small Fermi petals, and a change in the electronic periodicity from body-centred tetragonal to simple tetragonal. Our results explain the large entropy loss in the hidden-order phase, and the similarity between this phase and the high-pressure antiferromagnetic phase found in quantum-oscillation experiments.
Two-dimensional electron gases (2DEGs) forming at the interfaces of transition metal oxides exhibit a range of properties, including tunable insulator-superconductor-metal transitions, large magnetoresistance, coexisting ferromagnetism and superconductivity, and a spin splitting of a few meV (refs 10, 11). Strontium titanate (SrTiO3), the cornerstone of such oxide-based electronics, is a transparent, non-magnetic, wide-bandgap insulator in the bulk, and has recently been found to host a surface 2DEG (refs 12-15). The most strongly confined carriers within this 2DEG comprise two subbands, separated by an energy gap of 90 meV and forming concentric circular Fermi surfaces. Using spin- and angle-resolved photoemission spectroscopy (SARPES), we show that the electron spins in these subbands have opposite chiralities. Although the Rashba effect might be expected to give rise to such spin textures, the giant splitting of almost 100 meV at the Fermi level is far larger than anticipated. Moreover, in contrast to a simple Rashba system, the spin-polarized subbands are non-degenerate at the Brillouin zone centre. This degeneracy can be lifted by time-reversal symmetry breaking, implying the possible existence of magnetic order. These results show that confined electronic states at oxide surfaces can be endowed with novel, non-trivial properties that are both theoretically challenging to anticipate and promising for technological applications.
We study, using high-resolution angle-resolved photoemission spectroscopy, the evolution of the electronic structure in URu2Si2 at the Γ, Z, and X high-symmetry points from the high-temperature Kondo-screened regime to the low-temperature hidden-order (HO) state. At all temperatures and symmetry points, we find structures resulting from the interaction between heavy and light bands related to the Kondo-lattice formation. At the X point, we directly measure a hybridization gap of 11 meV already open at temperatures above the ordered phase. Strikingly, we find that while the HO induces pronounced changes at Γ and Z, the hybridization gap at X does not change, indicating that the hidden-order parameter is anisotropic. Furthermore, at the Γ and Z points, we observe the opening of a gap in momentum in the HO state, and show that the associated electronic structure results from the hybridization of a light electron band with the Kondo-lattice bands characterizing the paramagnetic state.