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Spatially controlling the Fermi level of topological insulators and keeping their electronic states stable are indispensable processes to put this material into practical use for semiconductor spintronics devices. So far, however, such a method has not been established yet. Here we show a novel method for doping a hole into n-type topological insulators Bi2X3 (X= Se, Te) that overcomes the shortcomings of the previous reported methods. The key of this doping is to adsorb H2O on Bi2X3 decorated with a small amount of carbon, and its trigger is the irradiation of a photon with sufficient energy to excite the core electrons of the outermost layer atoms. This method allows controlling the doping amount by the irradiation time and acts as photolithography. Such a tunable doping makes it possible to design the electronic states at the nanometer scale and, thus, paves a promising avenue toward the realization of novel spintronics devices based on topological insulators.

In the field of topological materials, the interaction between band topology and magnetism remains a current frontier for the advancement of new topological states and spintronic functionalities. D...

HgTe is a versatile topological material and has enabled the realization of a variety of topological states, including two- and three-dimensional (3D) topological insulators and topological semimetals. Nevertheless, a quantitative understanding of its electronic structure remains challenging, in particular due to coupling of the Te 5p-derived valence electrons to Hg 5d core states at shallow binding energy. We present a joint experimental and theoretical study of the electronic structure in strained HgTe(001) films in the 3D topological-insulator regime, based on angle-resolved photoelectron spectroscopy and density functional theory. The results establish detailed agreement in terms of (i) electronic band dispersions and orbital symmetries, (ii) surface and bulk contributions to the electronic structure, and (iii) the importance of Hg 5d states in the valence-band formation. Supported by theory, our experiments directly image the paradigmatic band inversion in HgTe, underlying its non-trivial band topology.

Disordered heterostructures stand as a general description for compounds that are part of homologous series such as bismuth chalcogenides. In device engineering, van der Waals epitaxy of these compounds is very promising for applications in spintronic and quantum computing. Structural analysis methods are essential to control and improve their synthesis in the form of thin films. Recently, X-rays tools have been proposed for structural modeling of disordered heterostructures [arXiv:2107.12280]. Here, we further evaluate the use of these tools to study the compound Mn$_x$Bi$_2$Te$_{3+x}$ in the grazing incidence region of the reflectivity curves, as well as the effect of thickness fluctuation in the wide angle region., 10 pages, 3 figures, and 1 table

Using angle-resolved photoelectron spectroscopy (ARPES), we investigate the surface electronic structure of the magnetic van der Waals compounds MnBi_{4}Te_{7} and MnBi_{6}Te_{10}, the n=1 and 2 members of a modular (Bi_{2}Te_{3})_{n}(MnBi_{2}Te_{4}) series, which have attracted recent interest as intrinsic magnetic topological insulators. Combining circular dichroic, spin-resolved and photon-energy-dependent ARPES measurements with calculations based on density functional theory, we unveil complex momentum-dependent orbital and spin textures in the surface electronic structure and disentangle topological from trivial surface bands. We find that the Dirac-cone dispersion of the topologial surface state is strongly perturbed by hybridization with valence-band states for Bi_{2}Te_{3}-terminated surfaces but remains preserved for MnBi_{2}Te_{4}-terminated surfaces. Our results firmly establish the topologically nontrivial nature of these magnetic van der Waals materials and indicate that the possibility of realizing a quantized anomalous Hall conductivity depends on surface termination.

We investigate the coupled spin and orbital textures of the topological surface state in ${\mathrm{Bi}}_{2}$(Te,${\mathrm{Se})}_{3}$(0001) across full momentum space using spin- and angle-resolved photoelectron spectroscopy and relativistic one-step photoemission theory. For an approximately isotropic Fermi surface in ${\mathrm{Bi}}_{2}{\mathrm{Te}}_{2}\mathrm{Se}$, the measured intensity and spin momentum distributions, obtained with linearly polarized light, qualitatively reflect the orbital composition and the orbital-projected in-plane spin polarization, respectively. In ${\mathrm{Bi}}_{2}{\mathrm{Te}}_{3}$, the in-plane lattice potential induces a hexagonal anisotropy of the Fermi surface, which manifests in an out-of-plane photoelectron spin polarization with a strong dependence on light polarization, excitation energy, and crystallographic direction.

A Correction to this paper has been published: https://doi.org/10.1038/s41535-021-00314-9

The combination of x-ray magnetic circular dichroism with multiplet ligand field theory is a powerful method to study magnetic ground state properties. Here, the authors use this approach to reveal a strongly covalent ferromagnetic ground state of V and Cr impurities embedded in Bi${}_{x}$Sb${}_{2\ensuremath{-}x}$Te${}_{3}$ topological-insulator thin films. They find a substantial charge transfer from the Te ligands to the impurities and a surprisingly negligible contribution from ionic V${}^{3+}$ and Cr${}^{3+}$. The authors also succeed in quantifying the magnetic moments and orbital occupations, which are key parameters for theories of the magnetic coupling mechanism.

Physical review / B 102(18), 184401 (1-13) (2020). doi:10.1103/PhysRevB.102.184401, Rare-earth ions typically exhibit larger magnetic moments than transition-metal ions and thus promise the opening of a wider exchange gap in the Dirac surface states of topological insulators. Yet in a recent photoemission study of Eu-doped Bi$_2$Te$_3$ films, the spectra remained gapless down to T=20 K. Here we scrutinize whether the conditions for a substantial gap formation in this system are present by combining spectroscopic and bulk characterization methods with theoretical calculations. For all studied Eu doping concentrations, our atomic multiplet analysis of the M$_{4,5}$ x-ray absorption and magnetic circular dichroism spectra reveals a Eu$^{2+}$ valence and confirms a large magnetic moment, consistent with a 4$f^7$$^8S$$_{7/2}$ ground state. At temperatures below 10 K, bulk magnetometry indicates the onset of antiferromagnetic (AFM) ordering. This is in good agreement with density functional theory, which predicts AFM interactions between the Eu impurities. Our results support the notion that antiferromagnetism can coexist with topological surface states in rare-earth-doped Bi$_2$Te$_3$ and call for spectroscopic studies in the Kelvin range to look for novel quantum phenomena such as the quantum anomalous Hall effect., Published by Inst., Woodbury, NY

Successful applications of a topological insulator (TI) in spintronics require its bandgap to be wider then in a typical TI and the energy position of the Dirac point in the dispersion relations to be away from the valence and conduction bands. In this study we grew Bi1.1Sb0.9Te2S crystals and examined their elemental composition, structural, optical and electronic properties as well as the electronic band structure. The high structural quality of the grown crystals was established by X-ray diffraction and Raman spectroscopy. Angular resolved photoelectron spectroscopy demonstrated a near parabolic character of the valence and conduction bands and a direct bandgap of 0.36 eV. The dispersion relations also revealed a Dirac cone, confirming the topological insulator nature of this material, with the position of the Dirac point being 100 meV above the valence band maximum. Far infrared reflectivity spectra revealed a plasma edge and two phonon dips. Fitting these spectra with theoretical functions based on the Drude-Lorentz model allows determination of the high frequency dielectric constant (41.3), plasma frequency (936 cm−1) and the frequencies of two infrared phonons (177.7 cm−1 and 77.4 cm−1). © 2021 Elsevier B.V. The reported study was funded by RFBR, project number 19-29-12061 . The part of optical research was carried out within the state assignment of Ministry of Science and Higher Education of the Russian Federation (theme "Spin" No AAAA-A18-118020290104-2 and No AAAA-A19-119081990020-8 and theme "Electron" No AAAAA18-118020190098-5 ). The study was also supported by the Russian Science Foundation (Project No. 17-12-01047 ) in the part of the crystal growth and state assignment of ISP SB RAS ( 0306–2019-0007 ) and IGM SB RAS. The Raman measurements were partially supported by the grant of the Russian Foundation for Basic Research (Project No. 19-52-18008 ). This work is funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) through project-ID 258499086 – SFB 1170 (A01), the Würzburg-Dresden Cluster of Excellence on Complexity and Topology in Quantum Matter–ct.qmat Project-ID 390858490 – EXC 2147 .

The Rashba effect is fundamental to the physics of two-dimensional electron systems and underlies a variety of spintronic phenomena. It has been proposed that the formation of Rashba-type spin splittings originates microscopically from the existence of orbital angular momentum (OAM) in the Bloch wave functions. Here, we present detailed experimental evidence for this OAM-based origin of the Rashba effect by angle-resolved photoemission (ARPES) and two-photon photoemission (2PPE) experiments for a monolayer AgTe on Ag(111). Using quantitative low-energy electron diffraction (LEED) analysis we determine the structural parameters and the stacking of the honeycomb overlayer with picometer precision. Based on an orbital-symmetry analysis in ARPES and supported by first-principles calculations, we unequivocally relate the presence and absence of Rashba-type spin splittings in different bands of AgTe to the existence of OAM.

The layered van der Waals antiferromagnet MnBi$_2$Te$_4$ has been predicted to combine the band ordering of archetypical topological insulators such as Bi$_2$Te$_3$ with the magnetism of Mn, making this material a viable candidate for the realization of various magnetic topological states. We have systematically investigated the surface electronic structure of MnBi$_2$Te$_4$(0001) single crystals by use of spin- and angle-resolved photoelectron spectroscopy experiments. In line with theoretical predictions, the results reveal a surface state in the bulk band gap and they provide evidence for the influence of exchange interaction and spin-orbit coupling on the surface electronic structure., Revised version

Chemistry of materials 31(8), 2795 - 2806 (2019). doi:10.1021/acs.chemmater.8b05017, High-quality single crystals of MnBi2Te4 are grown for the first time by slow cooling within a narrow range between the melting points of Bi$_2$Te$_3$ (586 °C) and MnBi$_2$Te$_4$ (600 °C). Single-crystal X-ray diffraction and electron microscopy reveal ubiquitous antisite defects in both cation sites and, possibly, Mn vacancies (Mn$_{0.85(3)}$Bi$_{2.10(3)}$Te$_4$). Thermochemical studies complemented with high-temperature X-ray diffraction establish a limited high-temperature range of phase stability and metastability at room temperature. Nevertheless, the synthesis of MnBi$_2$Te$_4$ can be scaled-up as powders can be obtained at subsolidus temperatures and quenched at room temperature. Bulk samples exhibit long-range antiferromagnetic ordering below 24 K. The Mn(II) out-of-plane magnetic state is confirmed by the magnetization, X-ray photoemission, X-ray absorption, and linear dichroism measurements. The compound shows a metallic type of resistivity in the range 4.5–300 K and is an n-type conductor that reaches a thermoelectric figure of merit up to ZT = 0.17. Angle-resolved photoemission experiments show a surface state forming a gapped Dirac cone, thus strengthening MnBi$_2$Te$_4$ as a promising candidate for the intrinsic magnetic topological insulator, in accordance with theoretical predictions. The developed synthetic protocols enable further experimental studies of a crossover between magnetic ordering and nontrivial topology in bulk MnBi$_2$Te$_4$., Published by American Chemical Society, Washington, DC

The layered van der Waals compounds ( MnBi 2 Te 4)( Bi 2 Te 3) were recently established as the first intrinsic magnetic topological insulators. We report a study on the epitaxial growth of ( MnBi 2 Te 4 ) m ( Bi 2 Te 3 ) n films based on the co-deposition of MnTe and Bi 2 Te 3 on BaF 2 (111) substrates. X-ray diffraction and scanning transmission electron microscopy evidence the formation of multilayers of stacked MnBi 2 Te 4 septuple layers and Bi 2 Te 3 quintuple layers with a predominance of MnBi 2 Te 4. The elemental composition and morphology of the films is further characterized by x-ray photoemission spectroscopy and atomic force microscopy. X-ray magnetic circular and linear dichroism spectra are comparable to those obtained for MnBi 2 Te 4 single crystals and confirm antiferromagnetic order in the films.

BaTiO${}_{3}$ (BTO) is one of the most important ferroelectric oxides. Its most common source of uncontrolled doping, the oxygen vacancy, releases free electrons that confine in a two-dimensional electron gas (2DEG) at the surface. This 2DEG can be readily monitored by angle-resolved photoemission, and be used to measure the defect dynamics in ultrathin BTO films. The authors reveal two remarkable properties: first, oxygen defects close to the thin film surface are preferably in a charge state of 2+, which limits charge carrier trapping. Second, these defects migrate even below room temperature, fostering significant surface charge carrier density fluctuations that ultimately quench the 2DEG.

The monopnictides TaAs and TaP are well-established Weyl semimetals. Yet, a precise assignment of Fermi arcs, accommodating the predicted chiral charge of the bulk Weyl points, has been difficult in these systems, and the topological character of different surface features in the Fermi surface is not fully understood. Here, employing a joint analysis from linear dichroism in angle-resolved photoemission and first-principles calculations, we unveil the orbital texture on the full Fermi surface of TaP(001). We observe pronounced switches in the orbital texture at the projected Weyl nodes, and show how they facilitate a topological classification of the surface band structure. Our findings establish a critical role of the orbital degrees of freedom in mediating the surface-bulk connectivity in Weyl semimetals.

The layered polar semiconductor BiTeI exhibits large Rashba-type spin–orbit splittings in its bulk and surface electronic structure. Here we report an artificial structural modification near the surface of BiTeI(0001) induced by annealing in vacuum. Using scanning tunneling microscopy we show that the annealing-induced change in the near-surface stoichiometry results in a structural change from a non-centrosymmetric triple-layered to a quintuple-layered structure. The structural change gives rise to the emergence of topological surface states with helical spin texture as demonstrated by angle-resolved photoemission experiments and relativistic first-principles calculations. The results provide a way to modify the electronic structure of layered materials by a controlled manipulation of the atomic stacking, This work was supported by the Deutsche Forschungsgemeinschaft through SFB1170 (project A01), and partly by the Tomsk State University competitiveness improvement programme (project No. 8.1.01.201 7), by the Russian Science Foundation (Grants No. 17-12-01047, in part of crystal growth and ARPES measurements (figure 4) and 18-12-00169, in part of DFT calculations), Russian Foundation for Basic Research (Grant No. 17- 02-00729) and Saint Petersburg State University (project 15.61.202.201 5).

The electronic structure of the Sb 2 Te 3 (0 0 0 1) surface exhibits a spin–orbit split surface state in a local energy gap of the projected bulk valence band continuum. We investigate this surface state by high-resolution angle-resolved photoemission spectroscopy (ARPES), spin-resolved ARPES and relativistic one-step photoemission calculations. At low wave vectors the dispersion and spin splitting are well-captured by the predictions of the Rashba model for a two-dimensional electron system. With increasing wave vectors, however, the surface state dispersion becomes more complex and the spin splitting size exhibits an unusual non-monotonic evolution. These deviations from the Rashba model arise from the influence of bulk continuum states near the edge of the projected gap. The spin polarization of the surface state remains intact despite the coupling to bulk states.

Paramagnetic heavy fermion insulators consist of fully occupied quasiparticle bands inherent to Fermi liquid theory. The gap emergence below a characteristic temperature is the ultimate sign of coherence for a many-body system, which in addition can induce a non-trivial band topology. Here, we demonstrate a simple and efficient method to compare a model study and an experimental result for heavy fermion insulators. The temperature dependence of the gap formation in both local moment and mixed valence regimes is captured within the dynamical mean field (DMFT) approximation to the periodic Anderson model (PAM). Using the topological coherence temperature as the scaling factor and choosing the input parameter set within the mixed valence regime, we can unambiguously link the theoretical energy scales to the experimental ones. As a particularly important result, we find improved consistency between the scaled DMFT density of states and the photoemission near-gap spectra of samarium hexaboride (SmB6).

A comprehensive understanding of spin-polarized photoemission is crucial for accessing the electronic structure of spin-orbit coupled materials. Yet, the impact of the final state in the photoemission process on the photoelectron spin has been difficult to assess in these systems. We present experiments for the spin-orbit split states in a Bi-Ag surface alloy showing that the alteration of the final state with energy may cause a complete reversal of the photoelectron spin polarization. We explain the effect on the basis of ab initio one-step photoemission theory and describe how it originates from linear dichroism in the angular distribution of photoelectrons. Our analysis shows that the modulated photoelectron spin polarization reflects the intrinsic spin density of the surface state being sampled differently depending on the final state, and it indicates linear dichroism as a natural probe of spin-orbit coupling at surfaces., New manuscript with a changed interpretation and theoretical description of the experimental results

As an avenue to spintronics, controlling spin-polarized electronic states in low-dimensional heterostructures is at the frontier of physics and nanotechnology. Manipulating these states via ferroelectric polarization seems promising, but actually making high-quality interfaces, to realize states with large spin splitting upon a ferroelectric substrate, remains tricky. The authors rise to the challenge, directly demonstrating metallic states with large spin splitting in the wide band gap of BaTiO${}_{3}$, with evidence for considerable coupling between overlayer and substrate.

The ferromagnetic topological insulator $\mathrm{V}:{(\mathrm{Bi},\mathrm{Sb})}_{2}{\mathrm{Te}}_{3}$ has been recently reported as a quantum anomalous Hall (QAH) system. Yet the microscopic origins of the QAH effect and the ferromagnetism remain unclear. One key aspect is the contribution of the V atoms to the electronic structure. Here the valence band of $\mathrm{V}:{(\mathrm{Bi},\mathrm{Sb})}_{2}{\mathrm{Te}}_{3}$ thin films was probed in an element-specific way by resonant photoemission spectroscopy. The signature of the V $3d$ impurity band was extracted and exhibits a high density of states near the Fermi level, in agreement with spin-polarized first-principles calculations. Our results indicate the occurrence of a ferromagnetic superexchange interaction mediated by the observed impurity band, contributing to the ferromagnetism in this system.

The photoelectron spin polarization in angle-resolved photoemission from the topological surface state in ${\mathrm{Bi}}_{2}{\mathrm{Te}}_{3}$(0001) has been investigated in a combined experimental and theoretical study. Our measurements show significant photon-energy-dependent deviations in the three-dimensional spin polarization of the photoelectron when compared to the expected intrinsic spin polarization of the surface state. The experimental observations are in line with relativistic one-step photoemission calculations. Our theoretical analysis confirms that spin-orbit coupling in the initial-state wave functions in combination with the dipole selection rules strongly influences the photoelectron spin polarization. Furthermore, spin-dependent final-state effects are found to influence the spin polarization significantly. A quantitative access to the three-dimensional spin-polarization vector in topological insulators is thus challenged by a complex interplay of initial- and final-state effects in the photoemission process.

Ex situ analyses on topological insulator films require protection against surface contamination during air exposure. This work reports on a technique that combines deposition of protective capping just after epitaxial growth and its mechanical removal inside ultra-high vacuum systems. This method was applied to Bi2Te3 films with thickness varying from 8 to 170 nm. Contrarily to other methods, this technique does not require any sputtering or thermal annealing setups installed inside the analyzing system and preserves both film thickness and surface characteristics. These results suggest that the technique presented here can be expanded to other topological insulator materials.

Semiconductors with strong spin–orbit interaction as the underlying mechanism for the generation of spin-polarized electrons are showing potential for applications in spintronic devices. Unveiling the full spin texture in momentum space for such materials and its relation to the microscopic structure of the electronic wave functions is experimentally challenging and yet essential for exploiting spin–orbit effects for spin manipulation. Here we employ a state-of-the-art photoelectron momentum microscope with a multichannel spin filter to directly image the spin texture of the layered polar semiconductor BiTeI within the full two-dimensional momentum plane. Our experimental results, supported by relativistic ab initio calculations, demonstrate that the valence and conduction band electrons in BiTeI have spin textures of opposite chirality and of pronounced orbital dependence beyond the standard Rashba model, the latter giving rise to strong optical selection-rule effects on the photoelectron spin polarization. These observations open avenues for spin-texture manipulation by atomic-layer and charge carrier control in polar semiconductors., This work was supported by DFG (through SFB 1170 ‘ToCoTronics’) and through FOR1162 (P3). We acknowledge the support by the Basque Departamento de Educacion, UPV/EHU (Grant Number IT-756-13), Spanish Ministerio de Economia y Competitividad (MINECO Grant Number FIS2013-48286-C2-2-P), Tomsk State University Academic D.I. Mendeleev Fund Program in 2015 (Research Grant Number 8.1.05.2015), the Russian Foundation for Basic Research (Grant Numbers 15-02-01797 and 15-02-589 02717). Partial support by the Saint Petersburg State University (Grant Number 15.61.202.2015) is also acknowledged.

The noncentrosymmetric semiconductors $\mathrm{BiTe}X\phantom{\rule{4pt}{0ex}}(X=\text{Cl},\text{Br},\text{I})$ show large Rashba-type spin-orbit splittings in their electronic structure making them candidate materials for spin-based electronics. However, BiTeI(0001) single-crystal surfaces usually consist of stacking-fault-induced domains of Te and I terminations implying a spatially inhomogeneous electronic structure. Here we combine scanning tunneling microscopy, photoelectron spectroscopy (ARPES, XPS), and density functional theory calculations to systematically investigate the structural and electronic properties of $\mathrm{BiTe}X(0001)$ surfaces. For $X=\text{Cl}$, Br we observe macroscopic single-terminated surfaces. We discuss chemical characteristics among the three materials in terms of bonding character, surface electronic structure, and surface morphology.

The surface state of a ${\mathbb{Z}}_{2}$ topological insulator connects with the conduction and valence band continua of the bulk, thereby bridging the band gap of the volume. We investigate this connection of the surface and bulk electronic structure for ${\mathrm{Sb}}_{2}{\mathrm{Te}}_{3}(0001)$ by photoemission experiments and calculations. Upon crossing the topmost valence band the topological surface state (TSS) maintains a coherent spectral signature, a two-dimensional character, and a linear dispersion relation. Surface-bulk coupling manifests itself in the spectra through (i) a characteristic kink in the TSS dispersion as it crosses the topmost valence band and (ii) the appearance of hybridization gaps between the TSS and bulk-derived surface resonance states at higher binding energies. The findings provide a natural explanation for the unexpectedly weak surface-bulk mixing indicated by recent transport experiments on ${\mathrm{Sb}}_{2}{\mathrm{Te}}_{3}$.

We present a detailed study on the temperature-dependence of the Sm 4 f states in mixed-valent samarium hexaboride (SmB 6 ) which, as a consequence of the hybridization with the conduction band states, largely determine the physical properties of the system. By comparing soft X-ray photoemission spectra of SmB 6 with those of Sm 0.35 La 0.65 B 6 , we discuss the apparent differences and similarities of the two systems. Based on our analyses we show that the 4 f spectra of SmB 6 can be separated into two independent spectral contributions with the 4 f peak maxima at different binding energies, representing two different electronic 4 f configurations existing in the system.

We report on the spectroscopic observation of a quantized electronic fine structure near the Fermi energy in thin Fe films grown on W(110). The quantum well states are detected down to binding energies of $\sim$10 meV by angle-resolved photoelectron spectroscopy. The band dispersion of these states is found to feature a pronounced anisotropy within the surface plane: It is free-electron like along the $\bar{\Gamma \rm{H}}$-direction while it becomes heavy along $\bar{\Gamma \rm{N}}$. Density functional theory calculations identify the observed states to have both majority and minority spin character and indicate that the large anisotropy can be dependent on the number of Fe-layers and coupling to the substrate., Comment: 5 pages, 5 figures

The surface state of a Z(2) topological insulator connects with the conduction and valence band continua of the bulk, thereby bridging the band gap of the volume. We investigate this connection of the surface and bulk electronic structure for Sb(2)Te(3)(0001) by photoemission experiments and calculations. Upon crossing the topmost valence band the topological surface state (TSS) maintains a coherent spectral signature, a two-dimensional character, and a linear dispersion relation. Surface-bulk coupling manifests itself in the spectra through (i) a characteristic kink in the TSS dispersion as it crosses the topmost valence band and (ii) the appearance of hybridization gaps between the TSS and bulk-derived surface resonance states at higher binding energies. The findings provide a natural explanation for the unexpectedly weak surface-bulk mixing indicated by recent transport experiments on Sb(2)Te(3).

Content from this work may be used under the terms of the Creative Commons Attribution 3.0 licence.-- et al., The surface electronic structure of the narrow-gap seminconductor BiTeI exhibits a large Rashba-splitting which strongly depends on the surface termination. Here we report on a detailed investigation of the surface morphology and electronic properties of cleaved BiTeI single crystals by scanning tunneling microscopy, photoelectron spectroscopy (ARPES, XPS), electron diffraction (SPA-LEED) and density functional theory calculations. Our measurements confirm a previously reported coexistence of Te- and I-terminated surface areas originating from bulk stacking faults and find a characteristic length scale of ∼100 nm for these areas. We show that the two terminations exhibit distinct types of atomic defects in the surface and subsurface layers. For electronic states resided on the I terminations we observe an energy shift depending on the time after cleavage. This aging effect is successfully mimicked by depositon of Cs adatoms found to accumulate on top of the I terminations. As shown theoretically on a microscopic scale, this preferential adsorbing behaviour results from considerably different energetics and surface diffusion lengths at the two terminations. Our investigations provide insight into the importance of structural imperfections as well as intrinsic and extrinsic defects on the electronic properties of BiTeI surfaces and their temporal stability., This work was financially supported by the Deutsche Forschungsgemeinschaft through FOR1162 and the Bundesministerium für Bildung und Forschung (grant numbers 05K10WW1/2 and 05KS1WMB/1). TVK and VIG acknowledge partial support from the Government of Sverdlovsk Region and Russian Foundation for Basic Research (grant no. 13-02-96046_Ural) and the Ural Branch of the Russian Academy of Sciences (grant no. 12-U-2-1002). This publication was funded by the Deutsche Forschungsgemeinschaft and the University of Würzburg in the funding programme Open Access Publishing.

The discovery of topologically non-trivial states in band insulators has induced an extensive search for topological phase in strongly correlated electron systems. In particular, samarium hexaboride (SmB$_6$) has drawn much attention as it might represent a new class of condensed matter called topological Kondo insulator. Kondo insulators (KI) can have non-trivial Z$_2$ topology because the energy gap opens at the Fermi energy ($E_F$) by hybridization between an odd- parity renormalized $f$ band and an even- parity conduction $d$ band. However, the characteristics of SmB$_6$ deviate from the conventional KI because its gap is insensitive to doping and pressure. Thus, it is unclear what makes the gap of SmB$_6$ different from that of KI, and how the band inversion features occur. In this manuscript, we demonstrate the importance of charge fluctuations in SmB$_6$. Our angle-resolved photoemission spectroscopy (ARPES) results reveal that with decreasing temperature the bottom of the $d$-$f$ hybridized band at the $\bar{\text{X}}$ point gradually shifts from below to above $E_F$. This shift accompanies a redistribution of spectral weight from the upper to the lower quasiparticle band, and reflects the change in both carrier density and the number of localized $f$ electron. Moreover, because this hybridized band is predicted to have odd parity and to induce a non-trivial $Z_{2}$ topology, we compare our ARPES spectra with theoretical surface band structures and find signatures of topological surface states. Therefore, our results indicate that SmB$_6$ is a charge fluctuating topological insulator having the odd-parity hybridized band above $E_F$ at the $X$ point. This demonstrates that the charge fluctuations do not only drive the insulating bulk phase but also the non-trivial topological phase., 12 pages, 5 figures

Using angle-resolved photoelectron spectroscopy we investigate the surface electronic structure of the three-dimensional topological insulator (TI) Sb${}_{2}$Te${}_{3}$(0001). Our data show the presence of a topological surface state in the bulk energy gap with the Dirac point located above the Fermi level. The adsorption of Cs atoms on Sb${}_{2}$Te${}_{3}$(0001) gives rise to a downward energy shift of the electronic valence band states which saturates at a value of $\ensuremath{\sim}$200 meV. For the saturation coverage the Dirac point of the linearly dispersive surface state resides in close proximity to the Fermi level. The electronic structure of the Cs/Sb${}_{2}$Te${}_{3}$ interface therefore considerably deviates from previously studied metal-TI interfaces based on the isostructural compound Bi${}_{2}$Se${}_{3}$ which points to the importance of atomic composition in these hetero systems.

We report the direct observation of interband spin-orbit (SO) coupling in a two-dimensional (2D) surface electron system, in addition to the anticipated Rashba spin splitting. Using angle-resolved photoemission experiments and first-principles calculations on Bi-Ag-Au heterostructures, we show that the effect strongly modifies the dispersion as well as the orbital and spin character of the 2D electronic states, thus giving rise to considerable deviations from the Rashba model. The strength of the interband SO coupling is tuned by the thickness of the thin film structures.

Whereas the magnitude of the Rashba spin splitting at surfaces has been studied in detail, less is known about its sign which determines the precise spin orientation of the electronic states. We investigate the microscopic origin of this sign by spin-resolved photoemission experiments and first-principles calculations on the strongly spin-orbit coupled surface states in Bi/Cu(111). We conclude that the sign of the Rashba splitting is determined by the particular charge asymmetry near the atomic cores. The precise spin orientation on heavy-element surfaces thus can comprise information on wave-function localizations and related aspects otherwise hardly accessible by other experimental methods. © 2011 American Physical Society.

We consider theoretically the early stages of the epitaxy of III-V compound semiconductors on high-index surfaces of elemental semiconductors. Specifically, we compare two models for the $7\ifmmode\times\else\texttimes\fi{}1$ indium-induced reconstruction of the silicon (112) surface. Density functional theory calculations suggest a substitutional model to be favorable when compared to on-terrace step edge adsorption in good agreement with recent low-electron-energy diffraction and scanning tunneling microscopy experiments. In addition, we report a comprehensive study of the atomic reconstruction and electronic structure of the (112) surfaces of group-IV semiconductors diamond, silicon, germanium, and $\ensuremath{\alpha}$-tin. We find the $1\ifmmode\times\else\texttimes\fi{}1$ rebonded reconstruction to be most stable for Si. For Ge and Sn the $2\ifmmode\times\else\texttimes\fi{}1$ reconstruction is most stable, and for carbon diamond it is $2\ifmmode\times\else\texttimes\fi{}2$. However, in all cases the mechanism of reconstruction is surprisingly similar to that known for the (001) surface.

We have studied by angle-resolved photoelectron spectroscopy the ordered XCu2 surface alloys formed by X=Sb and Bi on a Cu(111) substrate. We found clear analogies with the corresponding XAg2 alloys formed by the same elements on Ag(111). The electronic states near the Fermi level are similarly split by the spin-orbit (SO) interaction with the smaller splitting in XCu2 reflecting the smaller atomic SO parameter of Cu vs Ag. The charge transfer from the Bi and Sb adatoms to the substrate atoms and their outward relaxation are different for two substrates; both determine the Fermi energy of the two-dimensional electron gas.

A novel method is demonstrated to tailor the electronic structure of high-Z surface alloys showing a giant Rashba splitting by means of electron doping. This aims for new model systems to study unconvential spin topologies and for possible applications in the field of spintronics. We give new insights into the origin of the enhanced Rashba effect in the two specific alloys Bi/Cu(111) and Bi/Ag(111) employing angle-resolved photoelectron spectroscopy and first-principles calculations.

We report a theoretical and experimental study of thin Pt silicide films. Employing density-functional theory, we investigate the electronic structure, bonding, and optical properties of PtSi and ${\text{Pt}}_{2}\text{Si}$. Additionally, we calculate surface energies for various orientations and terminations of PtSi surfaces. Our results suggest that thermodynamics may play a role in the silicide formation. The complex dielectric function determined by spectroscopic ellipsometry exhibits non-Drude behavior and shows peaks, which are identified with interband transitions in the $5d$ manifold of platinum and compared with theory.

Epitaxial films of the ternary topological insulator Bi2Te2Se were grown on Si(111) substrates and investigated for their surface electronic properties and morphology. We employ a Se-capping procedure allowing for the preparation of clean films in the surface-analysis experimental setups. Using angle-resolved photoelectron spectroscopy, we determine the dispersion of the topological surface state. With time after surface preparation, the spectroscopic features in the surface electronic structure exhibit significant temperature-dependent shifts to higher binding energies. Scanning tunneling microscopy images show terraces with typical step edge separations of 50 nm–150 nm. X-ray photoelectron spectroscopy indicates an increased Se concentration at the surface.

Synthesis of new materials demands structural analysis tools suited to the particularities of each system. Van der Waals (vdW) materials are fundamental in emerging technologies of spintronics and quantum information processing, in particular topological insulators and, more recently, materials that allow the phenomenological exploration of the combination of non-trivial electronic band topology and magnetism. Weak vdW forces between atomic layers give rise to composition fluctuations and structural disorder that are difficult to control even in a typical binary topological insulators such as Bi2Te3. The addition of a third element as in MnBi2Te4 makes the epitaxy of these materials even more chaotic. In this work, statistical model structures of thin films on single crystal substrates are described. It allows the simulation of X-ray diffraction in disordered heterostructures, a necessary step towards controlling the epitaxial growth of these materials. On top of this, the diffraction simulation method described here can be readily applied as a general tool in the field of design new materials based on stacking of vdW bonded layers of distint elements., Comment: 12 pages, 9 figures