We study Na2IrO3 by angle-resolved photoemission spectroscopy, optics, and band structure calculations in the local-density approximation (LDA). The weak dispersion of the Ir 5d-t(2g) manifold highlights the importance of structural distortions and spin-orbit (SO) coupling in driving the system closer to a Mott transition. We detect an insulating gap Δ(gap)≃340  meV which, at variance with a Slater-type description, is already open at 300 K and does not show significant temperature dependence even across T(N)≃15  K. An LDA analysis with the inclusion of SO and Coulomb repulsion U reveals that, while the prodromes of an underlying insulating state are already found in LDA+SO, the correct gap magnitude can only be reproduced by LDA+SO+U, with U=3  eV. This establishes Na2IrO3 as a novel type of Mott-like correlated insulator in which Coulomb and relativistic effects have to be treated on an equal footing.

The electronic structure of Bi(2)Se(3) is studied by angle-resolved photoemission and density functional theory. We show that the instability of the surface electronic properties, observed even in ultrahigh-vacuum conditions, can be overcome via in situ potassium deposition. In addition to accurately setting the carrier concentration, new Rashba-like spin-polarized states are induced, with a tunable, reversible, and highly stable spin splitting. Ab initio slab calculations reveal that these Rashba states are derived from 5-quintuple-layer quantum-well states. While the K-induced potential gradient enhances the spin splitting, this may be present on pristine surfaces due to the symmetry breaking of the vacuum-solid interface.

Spin-orbit coupling has been conjectured to play a key role in the low-energy electronic structure of Sr 2 RuO 4 . By using circularly polarized light combined with spin-and angle-resolved photoemission spectroscopy, we directly measure the value of the effective spin-orbit coupling to be 130 AE 30 meV. This is even larger than theoretically predicted and comparable to the energy splitting of the d xy and d xz;yz orbitals around the Fermi surface, resulting in a strongly momentum-dependent entanglement of spin and orbital character in the electronic wavefunction. As demonstrated by the spin expectation value h ⃗ s k · ⃗ s −k i calculated for a pair of electrons with zero total momentum, the classification of the Cooper pairs in terms of pure singlets or triplets fundamentally breaks down, necessitating a description of the unconventional superconducting state of Sr 2 RuO 4 in terms of these newly found spin-orbital entangled eigenstates. DOI: 10.1103/PhysRevLett.112.127002 PACS numbers: 74.25.Jb, 74.20.Rp, 74.70.Pq, 79.60.-i After a flurry of experimental activity [1-5], Sr 2 RuO 4 has become a hallmark candidate for spin-triplet chiral p-wave superconductivity, the electronic analogue of superfluid 3 He [6][7][8]. However, despite the apparent existence of such a pairing, some later experiments [9-11] do not fully support this conclusion, as they cannot be explained within a theoretical model using spin-triplet superconductivity alone [12]. A resolution might come from the inclusion of spin-orbit (SO) coupling, which has been conjectured to play a key role in the normal-state electronic structure [13] and may be important when describing superconductivity as well. By mixing the canonical spin eigenstates, the relativistic SO interaction might play a fundamental role beyond simply lifting the degeneracy of competing pairing states [13][14][15][16][17].Thus far, the experimental study of SO coupling's effects on the electronic structure of Sr 2 RuO 4 has been limited to the comparison of band calculations against angle-resolved photoemission spectroscopy (ARPES) [13,[18][19][20][21] -no success has been obtained in observing experimentally either the strength of SO coupling or its implications for the mixing between spin and orbital descriptions. Here we probe this directly by performing spin-resolved ARPES [22], with circularly polarized light: by using the angular momentum inherent in each photon-along with electricdipole selection rules [23]-to generate spin-polarized photoemission from the SO mixed states. Combined with a novel spin-and orbitally-resolved ab initio based tightbinding (TB) modeling of the electronic structure [24], these results demonstrate the presence of a nontrivial spinorbital entanglement over much of the Fermi surface, i.e., with no simple way of factoring the band states into the spatial and spin sectors. Most importantly, the analysis of the corresponding Cooper pair spin eigenstates establishes the need for a description of the unconventional superconductivity of Sr 2 RuO 4 beyond...

By a combined angle-resolved photoemission spectroscopy and density functional theory study, we discover that the surface metallicity is polarity driven in SmB6. Two surface states, not accounted for by the bulk band structure, are reproduced by slab calculations for coexisting B6 and Sm surface terminations. Our analysis reveals that a metallic surface state stems from an unusual property, generic to the (001) termination of all hexaborides: the presence of boron 2p dangling bonds, on a polar surface. The discovery of polarity-driven surface metallicity sheds new light on the 40-year old conundrum of the low-temperature residual conductivity of SmB6, and raises a fundamental question in the field of topological Kondo insulators regarding the interplay between polarity and nontrivial topological properties.

We study the manipulation of the spin polarization of photoemitted electrons in Bi2Se3 by spin- and angle-resolved photoemission spectroscopy. General rules are established that enable controlling the photoelectron spin-polarization. We demonstrate the ± 100% reversal of a single component of the measured spin-polarization vector upon the rotation of light polarization, as well as full three-dimensional manipulation by varying experimental configuration and photon energy. While a material-specific density-functional theory analysis is needed for the quantitative description, a minimal yet fully generalized two-atomic-layer model qualitatively accounts for the spin response based on the interplay of optical selection rules, photoelectron interference, and topological surface-state complex structure. It follows that photoelectron spin-polarization control is generically achievable in systems with a layer-dependent, entangled spin-orbital texture.

We revisit the normal-state electronic structure of Sr(2)RuO(4) by angle-resolved photoemission spectroscopy with improved data quality, as well as ab initio band structure calculations in the local-density approximation with the inclusion of spin-orbit coupling. We find that the current model of a single surface layer (√2×√2)R45° reconstruction does not explain all detected features. The observed depth-dependent signal degradation, together with the close quantitative agreement with the slab calculations based on the surface crystal structure as determined by low-energy electron diffraction, reveal that-at a minimum-the subsurface layer also undergoes a similar although weaker reconstruction. This model accounts for all features-a key step in understanding the electronic structure-and indicates a surface-to-bulk progression of the electronic states driven by structural instabilities. Finally, we find no evidence for other phases stemming from either topological bulk properties or, alternatively, the interplay between spin-orbit coupling and the broken symmetry of the surface.

We report the thermodynamic and muon spin relaxation (µSR) evidences for a possible gapless spin liquid in Tm3Sb3Zn2O14, with the rare-earth ions Tm 3+ forming a two-dimensional kagomé lattice. We extract the magnetic specific heat of Tm3Sb3Zn2O14 by subtracting the phonon contribution of the non-magnetic isostructural material La3Sb3Zn2O14 and obtain a clear linear-T temperature dependence of magnetic specific heat at low temperatures. No long-range magnetic order was observed down to 0.35 K in the heat capacity measurements, and no signature of spin freezing down to 50 mK was observed in A.C. susceptibility measurements. The absence of magnetic order is further confirmed by the µSR measurements down to 20 mK. We find that the spinlattice relaxation time remains constant down to the lowest temperature. We point out that the physics in Tm3Sb3Zn2O14 is fundamentally different from the Cu-based herbertsmithite and propose spin liquid ground states with non-Kramers doublets on the kagomé lattice to account for the experimental results. However, we can not rule out that these exotic properties are induced by the Tm/Zn site-mixing disorder in Tm3Sb3Zn2O14.

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