As the size of a solid shrinks, the ratio of surface area to bulk volume grows and surface effect... more As the size of a solid shrinks, the ratio of surface area to bulk volume grows and surface effects become more important. In a world where technologies advance with the shrinking size of electronic devices, one phase of matter has emerged which is fit for the near future of surface-dominated performance. Moreover, it has brought a new set of ideas to solid-state physics and chemistry, especially the understanding that the discipline of topology can be applied to classify the electron band structures. The topological insulator phase yields an exotic metal surface state in which the orientation of the electron’s spin is locked perpendicular to its momentum. This property suppresses backscattering (making it possible to pass spin-polarized currents through the material without loss), offers a crucial ingredient for innovative approaches to quantum computation, and provides the basis for observing unique magnetoelectric effects. However, the surface states of materials in the topological insulator phase can wildly differ, so it is of interest to systematically characterize new materials to understand how the structure in position-space is related to the spin-resolved structure of electrons in energy- and momentum-space. We will discuss this relationship as it is probed through spin- and angle-resolved photoemission spectroscopy experiments on three topological (Bi2)m(Bi2Se3)n superlattices: (a) Bi2Se3 (m = 0, n = 1), (b) Bi4Se3 (m = 1, n = 1), and (c) BiSe (m = 1, n = 2). Our studies have not only proven the topological nature of these materials, but also demonstrate how bulk band structure and polar chemical bonding control the surface metal’s concentration, dispersion, and spin-orbital character. Case (a) is considered to provide an ideal model of the topological surface metal. Case (b) provides the three important findings: (1) the chemical identity of the surface-termination controls the orbital composition and energy distribution of the surface states, (2) there are two topological states in sequential bulk band gaps, (3) of these, one of topological state undergoes a hybridization effect that yields a momentum-dependent gap in the band structure as large as 85 meV. Case (c) has a practical significance in that the surface metal has a potentially record-breaking carrier density of ~10^13 cm^−2 (estimated from the Fermi surface area), more than an order of magnitude higher than in Bi2Se3. This occurs as a result of charge transfer from the Bi2 layers to the Bi2Se3 layers.
A three-dimensional strong-topological insulator or semimetal hosts topological surface states wh... more A three-dimensional strong-topological insulator or semimetal hosts topological surface states which are often said to be gapless so long as time-reversal symmetry is preserved. This narrative can be mistaken when surface state degeneracies occur away from time-reversal-invariant momenta. The mirror invariance of the system then becomes essential in protecting the existence of a surface Fermi surface. Here we show that such a case exists in the strong-topological-semimetal Bi4Se3. Angle-resolved photoemission spectroscopy and ab initio calculations reveal partial gapping of surface bands on the Bi2Se3 termination of Bi4Se3(111), where an 85 meV gap along ΓK closes to zero toward the mirror-invariant ΓM azimuth. The gap opening is attributed to an interband spin-orbit interaction that mixes states of opposite spin helicity.
A comparative study of the properties of topological insulator Bi2Te2Se (BTS) crystals grown by t... more A comparative study of the properties of topological insulator Bi2Te2Se (BTS) crystals grown by the vertical Bridgeman method is described. Two defect mechanisms that create acceptor impurities to compensate for the native n-type carriers are compared: Bi excess, and light Sn doping. Both methods yield low carrier concentrations and an n-p crossover over the length of the grown crystal boules, but lower carrier concentrations and higher resistivities are obtained for the Sn-doped crystals, which reach carrier concentrations as low as 8 x 1014 cm-3. Further, the temperature dependent resistivities for the Sn-doped crystals display strongly activated behavior at high temperatures, with a characteristic energy of half the bulk band gap. The (001) cleaved Sn-doped BTS crystals display high quality Shubnikov de Haas (SdH) quantum oscillations due to the topological surface state electrons. Angle resolved photoelectron spectroscopy (ARPES) characterization shows that the Fermi energy (EF) for the Sn-doped crystals falls cleanly in the surface states with no interference from the bulk bands, that the Dirac point for the surface states lies approximately 60 meV below the top of the bulk valence band maximum, and allows for a determination of the bulk and surface state carrier concentrations as a function of Energy near EF. Electronic structure calculations that compare Bi excess and Sn dopants in BTS demonstrate that Sn acts as a special impurity, with a localized impurity band that acts as a charge buffer occurring inside the bulk band gap. We propose that the special resonant level character of Sn in BTS gives rise to the exceptionally low carrier concentrations and activated resistivities observed.
Proximity-induced superconductivity in a 3D topological insulator represents a new avenue for obs... more Proximity-induced superconductivity in a 3D topological insulator represents a new avenue for observing zero-energy Majorana fermions inside vortex cores. Relatively small gaps and low transition temperatures of conventional s-wave superconductors put the hard constraints on these experiments. Significantly larger gaps and higher transition temperatures in cuprate superconductors might be an attractive alternative to considerably relax these constraints, but it is not clear whether the proximity effect would be effective in heterostructures involving cuprates and topological insulators. Here, we present angle-resolved photoemission studies of thin Bi2Se3 films grown in-situ on optimally doped Bi2Sr2CaCu2O8 substrates that show the absence of proximity-induced gaps on the surfaces of Bi2Se3 films as thin as a 1.5 quintuple layer. These results suggest that the superconducting proximity effect between a cuprate superconductor and a topological insulator is strongly suppressed, likely due to a very short coherence length along the c-axis, incompatible crystal and pairing symmetries at the interface, small size of the topological surface state Fermi surface and adverse effects of a strong spin-orbit coupling in the topological material.
Termination dependent topological surface states of the natural superlattice phase Bi4Se3
We describe the topological surface states of Bi$_4$Se$_3$, a compound in the infinitely adaptive... more We describe the topological surface states of Bi$_4$Se$_3$, a compound in the infinitely adaptive Bi$_2$-Bi$_2$Se$_3$ natural superlattice phase series, determined by a combination of experimental and theoretical methods. Two observable cleavage surfaces, terminating at Bi or Se, are characterized by angle resolved photoelectron spectroscopy and scanning tunneling microscopy, and modeled by ab-initio density functional theory calculations. Topological surface states are observed on both surfaces, but with markedly different dispersions and Kramers point energies. Bi$_4$Se$_3$ therefore represents the only known compound with different topological states on differently terminated surfaces.
Topological semimetal in a Bi Bi2Se3 infinitely adaptive superlattice phase
We report spin- and angle-resolved photoemission studies of a topological insulator from the infi... more We report spin- and angle-resolved photoemission studies of a topological insulator from the infinitely adaptive series between elemental Bi and Bi$_2$Se$_3$. The compound, based on Bi$_4$Se$_3$, is a 1:1 natural superlattice of alternating Bi$_2$ layers and Bi$_2$Se$_3$ layers; the inclusion of S allows the growth of large crystals, with the formula Bi$_4$Se$_{2.6}$S$_{0.4}$. The crystals cleave along the interfaces between the Bi$_2$ and Bi$_2$Se$_3$ layers, with the surfaces obtained having alternating Bi or Se termination. The resulting terraces, observed by photoemission electron microscopy, create avenues suitable for the study of one-dimensional topological physics. The electronic structure, determined by spin- and angle- resolved photoemission spectroscopy, shows the existence of a surface state that forms a large, hexagonally shaped Fermi surface around the $\Gamma$ point of the surface Brillouin zone, with the spin structure indicating that this material is a topological insulator.
Magnetic coupling of Fe-porphyrin molecules adsorbed on clean and c(2 × 2) oxygen-reconstructed Co(100) investigated by spin-polarized photoemission spectroscopy
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