Topological insulators are a novel materials platform with high applications potential in fields ranging from spintronics to quantum computation. In the ongoing scientific effort to demonstrate controlled manipulation of their electronic structure by
external means, stoichiometric variation and surface decoration are two effective approaches that have been followed. In ARPES experiments, both approaches are seen to lead to electronic band structure changes. Such approaches result in variations of the energy position of bulk and surface-related features and the creation of two-dimensional electron gases.The data presented here demonstrate that a third manipulation handle is accessible by utilizing the amount of illumination a topological insulator surface has been exposed to under typical experimental ARPES conditions. Our results show that this new, third, knob acts on an equal footing with stoichiometry and surface decoration as a modifier of the electronic band structure, and that it is in continuous competition with the latter. The data clearly point towards surface photovoltage and photo-induced desorption as the physical phenomena behind modifications of the electronic band structure under exposure to high-flux photons. We show that the interplay of these phenomena can minimize and even eliminate the adsorbate-related surface band bending on typical binary, ternary and quaternary Bi-based topological insulators. Including the influence of the sample temperature, these data set up a framework for the external control of the electronic band structure in topological insulator compounds in an ARPES setting. Four external knobs are available: bulk stoichiometry, surface decoration, temperature and photon exposure. These knobs can be used in conjunction to tune the band energies near the surface and consequently influence the topological properties of the relevant electronic states.
In an ideal 3D topological insulator (TI), the bulk is insulating and the surface conducting due to the existence of metallic states that are localized on the surface; these are the topological surface states. Quaternary Bi-based compounds of Bi$_{2-
x}$Sb$_{x}$Te$_{3-y}$Se$_{y}$ with finely-tuned bulk stoichiometries are good candidates for realizing ideal 3D TI behavior due to their bulk insulating character. However, despite its insulating bulk in transport experiments, the surface region of Bi$_{2-x}$Sb$_{x}$Te$_{3-y}$Se$_{y}$ crystals cleaved in ultrahigh vacuum also exhibits occupied states originating from the bulk conduction band. This is due to adsorbate-induced downward band-bending, a phenomenon known from other Bi-based 3D TIs. Here we show, using angle-resolved photoemission, how an EUV light beam of moderate flux can be used to exclude these topologically trivial states from the Fermi level of Bi$_{1.46}$Sb$_{0.54}$Te$_{1.7}$Se$_{1.3}$ single crystals, thereby re-establishing the purely topological character of the low lying electronic states of the system. We furthermore prove that this process is highly local in nature in this bulk-insulating TI, and are thus able to imprint structures in the spatial energy landscape at the surface. We illustrate this by `writing micron-sized letters in the Dirac point energy of the system.
We report high resolution Angle Resolved PhotoElectron Spectroscopy (ARPES) results on the (001) cleavage surface of YbB$_{6}$, a rare-earth compound which has been recently predicted to host surface electronic states with topological character. We o
bserve two types of well-resolved metallic states, whose Fermi contours encircle the time-reversal invariant momenta of the YbB$_{6}$(001) surface Brillouin zone, and whose full (E,$k$)-dispersion relation can be measured wholly unmasked by states from the rest of the electronic structure. Although the two-dimensional character of these metallic states is confirmed by their lack of out-of-plane dispersion, two new aspects are revealed in these experiments. Firstly, these states do not resemble two branches of opposite, linear velocity that cross at a Dirac point, but rather straightforward parabolas which terminate to high binding energy with a clear band bottom. Secondly, these states are sensitive to time-dependent changes of the YbB$_{6}$ surface under ultrahigh vacuum conditions. Adding the fact that these data from cleaved YbB$_{6}$ surfaces also display spatial variations in the electronic structure, it appears there is little in common between the theoretical expectations for an idealized YbB$_{6}$(001) crystal truncation on the one hand, and these ARPES data from real cleavage surfaces on the other.
SmB6, a well-known Kondo insulator, has been proposed to be an ideal topological insulator with states of topological character located in a clean, bulk electronic gap, namely the Kondo hybridisation gap. Seeing as the Kondo gap arises from many body
electronic correlations, this would place SmB6 at the head of a new material class: topological Kondo insulators. Here, for the first time, we show that the k-space characteristics of the Kondo hybridisation process is the key to unravelling the origin of the two types of metallic states observed directly by ARPES in the electronic band structure of SmB6(001). One group of these states is essentially of bulk origin, and cuts the Fermi level due to the position of the chemical potential 20 meV above the lowest lying 5d-4f hybridisation zone. The other metallic state is more enigmatic, being weak in intensity, but represents a good candidate for a topological surface state. However, before this claim can be substantiated by an unequivocal measurement of its massless dispersion relation, our data raises the bar in terms of the ARPES resolution required, as we show there to be a strong renormalisation of the hybridisation gaps by a factor 2-3 compared to theory, following from the knowledge of the true position of the chemical potential and a careful comparison with the predictions from recent LDA+Gutzwiler calculations. All in all, these key pieces of evidence act as triangulation markers, providing a detailed description of the electronic landscape in SmB6, pointing the way for future, ultrahigh resolution ARPES experiments to achieve a direct measurement of the Dirac cones in the first topological Kondo insulator.
The structural and electronic properties of thermally reduced SrTiO3(100) single crystals have been investigated using a probe with real- and reciprocal-space sensitivity: a synchrotron radiation microsopic setup which offers the possibility of Scann
ing Photoemission Microscopy and Angle Resolved Photoelectron Spectroscopy (ARPES) down to the nanometric scale. We have spectroscopically imaged the chemical composition of samples which present reproducible and suitable low-energy electron diffraction patterns after following well-established thermal reduction protocols. At the micrometric scale, Ca-rich areas have been directly imaged using high-energy resolution core level photoemission. Moreover, we have monitored the effect of Ca segregation on different features of the SrTiO3(100) electronic band structure, measuring ARPES inside, outside and at the interface of surface inhomogeneities with the identified Ca-rich areas. In particular, the interaction of Ca with the well-known intragap localized state, previously attributed to oxygen vacancies, has been investigated. Moreover, the combination of direct imaging and spectroscopic techniques with high spatial resolution has clarified the long-standing dilemma related to the bulk or surface character of Ca segregation in SrTiO3. Our results present solid evidence that the penetration depth of Ca segregation is very small. In contrast to what has been previously proposed, the origin of long-range surface reconstructions can unlikely be associated to Ca due to strong local variations of its surface concentration.
Spin polarized two-dimensional electronic states have been previously observed on metallic surface alloys with giant Rashba splitting and on the surface of topological insulators. We study the surface band structure of these systems, in a unified man
ner, by exploiting recent results of k.p theory. The model suggests a different way to address the effect of anisotropy in Rashba systems. Changes in the surface band structure of various Rashba compounds can be captured by a single effective parameter which quantifies the competition between the Rashba effect and the hexagonal warping of the constant energy contours. The same model provides a unified phenomenological description of the surface states belonging to materials with topologically trivial and non-trivial band structures.
We studied by angle-resolved photoelectron spectroscopy the strain-related structural transition from a pseudomorphic monolayer (ML) to a striped incommensurate phase in an Ag thin film grown on Pt(111). We exploited the surfactant properties of Bi t
o grow ordered Pt(111)-xMLAg-Bi trilayers with 0 < x < 5 ML, and monitored the dispersion of the Bi-derived interface states to probe the structure of the underlying Ag film. We find that their symmetry changes from threefold to sixfold and back to threefold in the Ag coverage range studied. Together with previous scanning tunneling microscopy and photoelectron diffraction data, these results provide a consistent microscopic description of the coverage-dependent structural transition.
The Bi/Si(111) (sqrt{3} x sqrt{3})R30 trimer phase offers a prime example of a giant spin-orbit splitting of the electronic states at the interface with a semiconducting substrate. We have performed a detailed angle-resolved photoemission (ARPES) stu
dy to clarify the complex topology of the hybrid interface bands. The analysis of the ARPES data, guided by a model tight-binding calculation, reveals a previously unexplored mechanism at the origin of the giant spin-orbit splitting, which relies primarily on the underlying band structure. We anticipate that other similar interfaces characterized by trimer structures could also exhibit a large effect.
