Search

Electronic structure of the 3x3 ordered-phase of a silicon (Si) layer on Al(111) has been studied by angle resolved photoemission spectroscopy (ARPES) technique using synchrotron radiation and modeled by a trial atomic model. A closed Fermi surface originating from linearly dispersing band is identified. A band structure calculation of a trial atomic model of the honeycomb silicene on Al(111) implies that the metallic band originates from the Al-Si hybrid state that has the Dirac cone-like dispersion curves. The Si layer on Al(111) can be a model system of Xene to realize the massless electronic system through the overlayer-substrate interaction., Comment: 6 pages, 6 figures

A paradigmatic case of multi-band Mott physics including spin-orbit and Hund's coupling is realised in Ca$_2$RuO$_4$. Progress in understanding the nature of this Mott insulating phase has been impeded by the lack of knowledge about the low-energy electronic structure. Here we provide -- using angle-resolved photoemission electron spectroscopy -- the band structure of the paramagnetic insulating phase of Ca$_2$RuO$_4$ and show how it features several distinct energy scales. Comparison to a simple analysis of atomic multiplets provides a quantitative estimate of the Hund's coupling $J=0.4$ eV. Furthermore, the experimental spectra are in good agreement with electronic structure calculations performed with Dynamical Mean-Field Theory. The crystal field stabilisation of the d$_{xy}$ orbital due to $c$-axis contraction is shown to be important in explaining the nature of the insulating state. It is thus a combination of multiband physics, Coulomb interaction and Hund's coupling that generates the Mott insulating state of Ca$_2$RuO$_4$. These results underscore the importance of Hund's coupling in the ruthenates and related multiband materials.

Thermoelectric (TE) devices have been attracting increasing attention because of their ability to convert heat directly to electricity. To date, improving the TE figure of merit remains the key challenge. The advent of the topological insulator and the emerging nanotechnology open a new way to design high-performance TE devices. In this paper, we investigate the TE transport properties of the Bi2Se3 thin film by the first-principle calculations and the Boltzmann transport theory. By comparing our calculations with the earlier experimental data, we demonstrate that, for the Bi2Se3 film of thickness larger than six quintuple layers, the relaxation time of the topological surface states in the bulk gap is about hundreds of femtoseconds, which is about two orders larger than that of the bulk states. Such a large relaxation-time difference causes the ratio of the electrical conductance to the thermal conductance much larger than the value predicted by the Wiedemann-Franz law, as well as the large magnitude of Seebeck coefficient, and consequently the large TE figure of merit, when the Fermi level is near the conduction band edge. We shows that the TE performance can be further improved by introducing defects in the middle layers of the thin film. The improvement is generally significant at room temperature and can be further enhanced at higher temperature., Comment: 19 pages 5 figures, and 6 pages 3 figures supplement

The first known magnetic mineral, magnetite (Fe$_3$O$_4$), has unusual properties which have fascinated mankind for centuries; it undergoes the Verwey transition at $T_{\rm V}$ $\sim$120 K with an abrupt change in structure and electrical conductivity. The mechanism of the Verwey transition however remains contentious. Here we use resonant inelastic X-ray scattering (RIXS) over a wide temperature range across the Verwey transition to identify and separate out the magnetic excitations derived from nominal Fe$^{2+}$ and Fe$^{3+}$ states. Comparison of the RIXS results with crystal-field multiplet calculations shows that the spin-orbital $dd$ excitons of the Fe$^{2+}$ sites arise from a tetragonal Jahn-Teller active polaronic distortion of the Fe$^{2+}$O$_6$ octahedra. These low-energy excitations, which get weakened for temperatures above 350 K but persist at least up to 550 K, are distinct from optical excitations and best explained as magnetic polarons.

A topological Dirac semimetal is a novel state of quantum matter which has recently attracted much attention as an apparent 3D version of graphene. In this paper, we report critically important results on the electronic structure of the 3D Dirac semimetal Na3Bi at a surface that reveals its nontrivial groundstate. Our studies, for the first time, reveal that the two 3D Dirac cones go through a topological change in the constant energy contour as a function of the binding energy, featuring a Lifshitz point, which is missing in a strict 3D analog of graphene (in other words Na3Bi is not a true 3D analog of graphene). Our results identify the first example of a band saddle point singularity in 3D Dirac materials. This is in contrast to its 2D analogs such as graphene and the helical Dirac surface states of a topological insulator. The observation of multiple Dirac nodes in Na3Bi connecting via a Lifshitz point along its crystalline rotational axis away from the Kramers point serves as a decisive signature for the symmetry-protected nature of the Dirac semimetal's topological groundstate., Comment: 5 pages, 4 Figures, Related papers on topological Fermi arcs and Weyl Semimetals (WSMs) are at http://physics.princeton.edu/zahidhasangroup/index.html

Symmetry or topology protected Dirac fermion states in two and three dimensions constitute novel quantum systems that exhibit exotic physical phenomena. However, none of the studied spin-orbit materials are suitable for realizing bulk multiplet Dirac states for the exploration of interacting Dirac physics. Here we present experimental evidence, for the first time, that the compound Na3Bi hosts a bulk spin-orbit Dirac multiplet and their interaction or overlap leads to a Lifshitz transition in momentum space - a condition for realizing interactions involving Dirac states. By carefully preparing the samples at a non-natural-cleavage (100) crystalline surface, we uncover many novel electronic and spin properties in Na3Bi by utilizing high resolution angle- and spin-resolved photoemission spectroscopy measurements. We observe two bulk 3D Dirac nodes that locate on the opposite sides of the bulk zone center point $\Gamma$, which exhibit a Fermi surface Lifshitz transition and a saddle point singularity. Furthermore, our data shows evidence for the possible existence of theoretically predicted weak 2D nontrivial spin-orbit surface state with helical spin polarization that are nestled between the two bulk Dirac cones, consistent with the theoretically calculated (100) surface-arc-modes. Our main experimental observation of a rich multiplet of Dirac structure and the Lifshitz transition opens the door for inducing electronic instabilities and correlated physical phenomena in Na3Bi, and paves the way for the engineering of novel topological states using Na3Bi predicted in recent theory., Comment: 23 pages, 5 Figures

Experimental identification of three-dimensional (3D) Dirac semimetals in solid state systems is critical for realizing exotic topological phenomena and quantum transport such as the Weyl phases, high temperature linear quantum magnetoresistance and topological magnetic phases. Using high resolution angle-resolved photoemission spectroscopy, we performed systematic electronic structure studies on well-known compound Cd3As2. For the first time, we observe a highly linear bulk Dirac cone located at the Brillouin zone center projected onto the (001) surface which is consistent with a 3D Dirac semimetal phase in Cd3As2. Remarkably, an unusually high Dirac Fermion velocity up to 10.2 \textrm{\AA}{\cdot}$eV (1.5 \times 10^{6} ms^-1) is seen in samples where the mobility far exceeds 40,000 cm^2/V.s suggesting that Cd3As2 can be a promising candidate as a hypercone analog of graphene in many device-applications which can also incorporate topological quantum phenomena in a large gap setting. Our experimental identification of this novel topological 3D Dirac semimetal phase, distinct from a 3D topological insulator phase discovered previously, paves the way for exploring higher dimensional relativistic physics in bulk transport and for realizing novel Fermionic matter such as a Fermi arc nodal metal., Comment: 4+ pages, 4 Figures, originally submitted in September (2013); Topological version was published at http://www.sciencemag.org/content/347/6219/294.full (Xu et.al., ScienceExpress 2014)

Quantitative understanding of the relationship between quantum tunneling and Fermi surface spin polarization is key to device design using topological insulator surface states. By using spin-resolved photoemission spectroscopy with p-polarized light in topological insulator Bi2Se3 thin films across the metal-to-insulator transition, we observe that for a given film thickness, the spin polarization is large for momenta far from the center of the surface Brillouin zone. In addition, the polarization decreases significantly with enhanced tunneling realized systematically in thin insulating films, whereas magnitude of the polarization saturates to the bulk limit faster at larger wavevectors in thicker metallic films. Our theoretical model calculations capture this delicate relationship between quantum tunneling and Fermi surface spin polarization. Our results suggest that the polarization current can be tuned to zero in thin insulating films forming the basis for a future spin-switch nano-device., Comment: 8 pages, 4 figures

The Kondo insulator SmB6 has long been known to exhibit low temperature (T < 10K) transport anomaly and has recently attracted attention as a new topological insulator candidate. By combining low-temperature and high energy-momentum resolution of the laser-based ARPES technique, for the first time, we probe the surface electronic structure of the anomalous conductivity regime. We observe that the bulk bands exhibit a Kondo gap of 14 meV and identify in-gap low-lying states within a 4 meV window of the Fermi level on the (001)-surface of this material. The low-lying states are found to form electron-like Fermi surface pockets that enclose the X and the Gamma points of the surface Brillouin zone. These states disappear as temperature is raised above 15K in correspondence with the complete disappearance of the 2D conductivity channels in SmB6. While the topological nature of the in-gap metallic states cannot be ascertained without spin (spin-texture) measurements our bulk and surface measurements carried out in the transport-anomaly-temperature regime (T < 10K) are consistent with the first-principle predicted Fermi surface behavior of a topological Kondo insulator phase in this material., Comment: 4 Figures, 6 Pages

The surface of topological insulators is proposed as a promising platform for spintronics and quantum information applications. In particular, when time- reversal symmetry is broken, topological surface states are expected to exhibit a wide range of exotic spin phenomena for potential implementation in electronics. Such devices need to be fabricated using nanoscale artificial thin films. It is of critical importance to study the spin behavior of artificial topological MBE thin films associated with magnetic dopants, and with regards to quantum size effects related to surface-to-surface tunneling as well as experimentally isolate time-reversal breaking from non-intrinsic surface electronic gaps. Here we present observation of the first (and thorough) study of magnetically induced spin reorientation phenomena on the surface of a topological insulator. Our results reveal dramatic rearrangements of the spin configuration upon magnetic doping contrasted with chemically similar nonmagnetic doping as well as with quantum tunneling phenomena in ultra-thin high quality MBE films. While we observe that the spin rearrangement induced by quantum tunneling occurs in a time-reversal invariant fashion, we present critical and systematic observation of an out-of-plane spin texture evolution correlated with magnetic interactions, which breaks time-reversal symmetry, demonstrating microscopic TRB at a Kramers' point on the surface., Comment: 12 pages, 3 Figures, Related results at http://online.kitp.ucsb.edu/online/topomat11/hasan/oh/01.html

Using angle-resolved photoemission spectroscopy, we report electronic structure for representative members of ternary topological insulators. We show that several members of this family, such as Bi2Se2Te, Bi2Te2Se, and GeBi2Te4, exhibit a singly degenerate Dirac-like surface state, while Bi2Se2S is a fully gapped insulator with no measurable surface state. One of these compounds, Bi2Se2Te, shows tunable surface state dispersion upon its electronic alloying with Sb (SbxBi2-xSe2Te series). Other members of the ternary family such as GeBi2Te4 and BiTe1.5S1.5 show an in-gap surface Dirac point, the former of which has been predicted to show nonzero weak topological invariants such as (1;111); thus belonging to a different topological class than BiTe1.5S1.5. The measured band structure presented here will be a valuable guide for interpreting transport, thermoelectric, and thermopower measurements on these compounds. The unique surface band topology observed in these compounds contributes towards identifying designer materials with desired flexibility needed for thermoelectric and spintronic device fabrication., Comment: 9 pages, 6 figures; Related results at http://online.kitp.ucsb.edu/online/topomat11/hasan/

Based on measurements of angle resolved photoemission, we report that in the Pb/Ge(111)- \sqrt{3}x\sqrt{3} R30^\circ structure, in addition to three bands resembling Ge heavy hole (HH), light hole (LH), and split off (SO) bulk band edges, a fourth dispersive band resembling the non split off (NSO) band is found near the surface zone center. While three Ge bulk-like bands get distorted due to strong coupling between Pb and Ge, the NSO-like band gets weaker and disappears for larger thickness of Pb, which, when combined with ab initio calculations, indicates its localized nature within space charge layer. Our results are clearly important for designing electronics involved with metal-semiconductor contacts., Comment: 21 pages, 4 figures, Phys. Rev. B 81, 245406 (2010)

X-ray absorption spectroscopy (XAS), optical reflectance spectroscopy, and the Hall effect measurements were used to investigate the electronic structure in La_0.7Ce_0.3MnO_3 thin films (LCeMO). The XAS results are consistent with those obtained from LDA+U calculations. In that the doping of Ce has shifted up the Fermi level and resulted in marked shrinkage of hole pockets originally existing in La_0.7Ca_0.3MnO_3 (LCaMO). The Hall measurements indicate that in LCeMO the carriers are still displaying the characteristics of holes as LDA+U calculations predict. Analyses of the optical reflectance spectra evidently disapprove the scenario that the present LCeMO might have been dominated by the La-deficient phases., Comment: 4 pages; Physical Review B, in press