For the purpose of recovering the intriguing electronic properties of freestanding graphene at a solid surface, graphene self-organized on a Au monolayer on Ni(111) is prepared and characterized by scanning tunneling microscopy. Angle-resolved photoemission reveals a gapless linear pi-band dispersion near K[over] as a fingerprint of strictly monolayer graphene and a Dirac crossing energy equal to the Fermi energy (EF) within 25 meV meaning charge neutrality. Spin resolution shows a Rashba effect on the pi states with a large (approximately 13 meV) spin-orbit splitting up to EF which is independent of k.

Understanding and control of spin degrees of freedom on the surfaces of topological materials are the key to future applications as well as for realizing novel physics such as the axion electrodynamics associated with time-reversal symmetry breaking on the surface. We experimentally demonstrate magnetically induced spin reorientation phenomena simultaneous with a Dirac-metal to gapped-insulator transition on the surfaces of manganese-doped Bi 2 Se 3 thin films. The resulting electronic groundstate exhibits unique hedgehog-like spin textures at low energies which directly demonstrates the mechanics of timereversal symmetry breaking on the surface. We further show that an insulating gap induced by quantum tunneling between surfaces exhibits spin texture modulation at low energies but respects time-reversal invariance. These spin phenomena and the control of their Fermi surface geometrical phase first demonstrated in our experiments pave the way for future realization of many predicted exotic magnetic phenomena of topological origin.Since the discovery of three dimensional topological insulators [1][2][3][4][5], topological order proximity to ferromagnetism has been considered as one of the core interests of the field [6][7][8][9][10][11][12][13][14][15][16]. Such interest is strongly motivated by the proposed time-reversal (TR) breaking topological physics such as quantized anomalous chiral Hall current, spin current, axion electrodynamics, and inverse spin-galvanic effect [9][10][11][12], all of which critically rely on finding a way to break TR symmetry on the surface and utilize the unique TR broken spin texture for applications. Since quantum coherence is essential in many of these applications, devices need to be engineered into thin films in order to enhance or de-enhance surface-tosurface coupling or the quantum tunneling of the electrons. The experimental spin behavior of surface states under the two extreme limits, namely the doped magnetic groundstate and ultra-thin film quantum tunneling groundstate, is thus of central importance to the entire field. However, surprisingly, it is not known what happens to the spin configuration under these extreme conditions relevant for device fabrications. Fundamentally, TR symmetry is inherently connected to the Kramers' degeneracy theorem which states that when TR symmetry is preserved, the electronic states at the TR invariant momenta have to remain doubly spin degenerate. Therefore, the establishment of TR breaking effect fundamentally requires measurements of electronic groundstate with a spin-sensitive probe. Here we utilize spin-3 resolved angle-resolved photoemission spectroscopy to measure the momentum space spin configurations in systematically magnetically doped, non-magnetically doped, and ultra-thin quantum coherent topological insulator films [17], in order to understand the nature of electronic groundstates under two extreme limits vital for magnetic topological devices. These measurements allow us to make definitive conclusions regarding magnetism on to...

Surfaces and interfaces o er new possibilities for tailoring the many-body interactions that dominate the electrical and thermal properties of transition metal oxides 1-4 . Here, we use the prototypical two-dimensional electron liquid (2DEL) at the SrTiO 3 (001) surface 5-7 to reveal a remarkably complex evolution of electron-phonon coupling with the tunable carrier density of this system. At low density, where superconductivity is found in the analogous 2DEL at the LaAlO 3 /SrTiO 3 interface 8-13 , our angle-resolved photoemission data show replica bands separated by 100 meV from the main bands. This is a hallmark of a coherent polaronic liquid and implies long-range coupling to a single longitudinal optical phonon branch. In the overdoped regime the preferential coupling to this branch decreases and the 2DEL undergoes a crossover to a more conventional metallic state with weaker short-range electron-phonon interaction. These results place constraints on the theoretical description of superconductivity and allow a unified understanding of the transport properties in SrTiO 3 -based 2DELs.Carrier concentration is a key parameter defining the ground state of correlated electron systems. At the LaAlO 3 /SrTiO 3 interface, the 2DEL density can be tailored by field-effect gating. As the system is depleted of carriers, its ground state evolves from a high-mobility 2DEL 4 into a two-dimensional superconductor 8-10 with pseudogap behaviour 11 and possible pairing above T c (ref. 12). An analogous 2DEL can be induced by doping the (001) surface of SrTiO 3 . As for the interface, the surface 2DEL is confined by a band-bending potential in SrTiO 3 and consists of an orbitally polarized ladder of quantum confined Ti t 2g electrons that are highly mobile in the surface plane [5][6][7]14 . Thus far, the surface 2DEL has been studied only at carrier densities around 2 × 10 14 cm −2 , approximately a factor of five higher than typically observed at the LaAlO 3 /SrTiO 3 interface [5][6][7] . In the following, we present ARPES data extending to lower carrier densities that are directly comparable to the LaAlO 3 /SrTiO 3 interface. We achieve this by preparing SrTiO 3 (001) wafers in situ, which results in well-ordered clean surfaces that can be studied by ARPES over extended timescales, as they are less susceptible to the ultraviolet-induced formation of charged oxygen vacancies reported for cleaved SrTiO 3 5,7,15,16 . Details of the sample preparation are given in Methods. Figure 1a shows an energy-momentum intensity map for a 2DEL with a carrier density of n 2D ≈ 2.9 × 10 13 cm −2 estimated from the Luttinger volume of the first light subband and the two equivalent heavy subbands (see Supplementary Section 2). The most striking features of this data are replica bands at higher binding energy following the dispersion of the primary quasiparticle (QP) bands. The replica bands are all separated by approximately 100 meV and progressively lose intensity, but can be visualized up to the third replica in the curvature plot shown in Fi...

Topological insulators 1-8 are a novel form of matter which features metallic surface states with quasirelativistic dispersion similar to graphene 9 . Unlike graphene, the locking of spin and momentum and the protection by time-reversal symmetry 1-8 open up tremendous additional possibilities for external control of transport properties 10-18 .Here we show by angle-resolved photoelectron spectroscopy that the topological surface states of Bi 2 Te 3 and Bi 2 Se 3 are stable against the deposition of Fe without opening a band gap. This stability extends to low submonolayer coverages meaning that the band gap reported recently 19 for Fe on Bi 2 Se 3 is incorrect as well as to complete monolayers meaning that topological surface states can very well exist at interfaces with ferromagnets in future devices.

A comprehensive mapping of the spin polarization of the electronic bands in ferroelectric α-GeTe(111) films has been performed using a time-of-flight momentum microscope equipped with an imaging spin filter that enables a simultaneous measurement of more than 10.000 data points (voxels). A Rashba type splitting of both surface and bulk bands with opposite spin helicity of the inner and outer Rashba bands is found revealing a complex spin texture at the Fermi energy. The switchable inner electric field of GeTe implies new functionalities for spintronic devices. The strong coupling of electron momentum and spin in low-dimensional structures allows an electrically controlled spin manipulation in spintronic devices [1-4], e.g. via the Rashba effect [5]. The Rashba effect has first been experimentally demonstrated in semiconductor heterostructures, where an electrical field perpendicular to the layered structure, i.e. perpendicular to the electron momentum, determines the electron spin orientation relative to its momentum [6-8]. An asymmetric interface structure causes the necessary inversion symmetry breaking and accounts for the special spin-splitting of electron states, the Rashba effect [5], the size of which can be tuned by the strength of the electrical field. For most semiconducting materials the Rashba effect causes only a quite small splitting of the order of 10 −2 ˚ A −1 and thus requires experiments at very low temperatures [9-11] and also implies large lateral dimensions for potential spintronic applications. A considerably larger splitting has been predicted theoretically [12] and was recently found experimentally for the surface states of GeTe(111) [13, 14]. GeTe is a ferroelectric semiconductor with a Curie temperature of 700 K. Thus, besides the interface induced Rashba splitting, the ferroelectric properties also imply a broken inversion symmetry within the bulk and thus would allow for the electrical tuning of the bulk Rashba splitting via switching the ferroelectric polarization [12, 15, 16]. This effect is of great interest for non-volatile spin orbitronics [10]. For GeTe a bulk Rashba splitting of 0.19Å19Å −1 has been predicted theoretically [12]. Experimentally, bulk-Rashba bands are rare and have only been found in the layered polar semiconductors BiTeCl and BiTeI [17-20] that, however, are not switchable. A characterization of the ferroelectric properties and a measurement of the spin polarization of the surface states of GeTe(111) at selected k-points has been performed previously by force microscopy [21, 22] and spin-resolved angular resolved photoemission spectroscopy, respectively [13]. A recent experimental and theoretical study revealed that at the Fermi level the hybridization of surface and bulk states causes surface-bulk resonant states resulting in unconventional spin topologies with chiral symmetry [14]. Here, we demonstrate the spin structure of surface and bulk bands of the GeTe(111) surface using the novel pho-toemission technique of spin-resolved time-of-flight momentum microsco...

Magnetically doped topological insulators enable the quantum anomalous Hall effect (QAHE) which provides quantized edge states for lossless charge transport applications [1][2][3][4][5][6][7][8][9]. The edge states are hosted by a magnetic energy gap at the Dirac point[2] but all attempts to observe it directly have been unsuccessful. The size of this gap is considered the clue to overcoming the present limitations of the QAHE, which so far occurs only at temperatures one to two orders of magnitude below its principle limit set by the ferromagnetic Curie temperature T C [8,9]. Here, we use low temperature photoelectron spectroscopy to unambiguously reveal the magnetic gap of Mn-doped Bi 2 Te 3 films which is present only below T C . Surprisingly, the gap turns out to be ∼ 90 meV wide, which not only exceeds k B T at room temperature but is also 5 times larger than predicted by density functional theory [10]. By an exhaustive multiscale structure characterization we show that this enhancement is due to a remarkable structure modification induced by Mn doping. Instead of a disordered impurity system, it forms an alternating sequence of septuple and quintuple layer blocks, where Mn is predominantly incorporated in the center of the septuple layers. This self-organized heterostructure substantially enhances the wave-function overlap and the size of the magnetic gap at the Dirac point, as recently predicted [11]. Mn-doped Bi 2 Se 3 forms a similar heterostructure, however, only a large, albeit nonmagnetic gap is formed. We explain both differences based on the higher spin-orbit interaction in Bi 2 Te 3 with the most important consequence of a magnetic anisotropy perpendicular to the films, whereas for Bi 2 Se 3 the spin-orbit interaction it is too weak to overcome the dipole-dipole interaction. Our findings provide crucial insights for pushing the lossless transport properties of topological insulators towards room-temperature applications.We thank B. Henne, F. Wilhelm, and A. Rogalev for support of the XANES and EX-AFS measurements at ID 12 and BM23 beam lines of the ESRF, V. Holý for advices on the structure model, W. Grafeneder for the TEM sample preparation and G. Bihlmayer and A. Ernst for helpful discussions. S.A.K and J.M. are grateful for support from CEDAMNF (CZ.02.1.01/0.0/0.0/15 003/0000358) of Czech ministry MSMT.

We reveal a giant Rashba effect ( R % 1:3 eV # A) on a surface state of Ir(111) by angle-resolved photoemission and by density functional theory. It is demonstrated that the existence of the surface state, its spin polarization, and the size of its Rashba-type spin-orbit splitting remain unaffected when Ir is covered with graphene. The graphene protection is, in turn, sufficient for the spin-split surface state to survive in ambient atmosphere. We discuss this result along with indications for a topological protection of the surface state. DOI: 10.1103/PhysRevLett.108.066804 PACS numbers: 73.22.Pr, 71.70.Ej, 73.20.At, 79.60.Dp The Rashba effect is based on symmetry breaking [1]: In the bulk of crystallographically inversion symmetric solids the time-reversal symmetry results in degenerate spin subbands of electronic valence states. At crystal surfaces or interfaces this structural inversion symmetry is broken and the spin degeneracy is lifted. A gradient of the electric potential perpendicular to the surface will then lead to a Rashba effect in two-dimensional systems with large spinorbit coupling [2]. It emerges as a splitting of the band structure into subbands E AE ðk k Þ of opposite spin which are displaced by electron wave vectors AEÁk k in opposite directions in momentum space. Regarding the transport properties of the solid this leads to the generation of dissipationless spin currents without the necessity for ferromagnetic materials or magnetic fields [3,4].In the quantum-mechanical description of a twodimensionally confined electron gas, the Rashba effect is accounted for by the Hamiltonianwhere denotes Pauli spin matrices and the parameter R is proportional to the potential gradient rV in the z direction and accounts for the size of the spin-orbit interaction. For free electrons, the two spin-split bands E AE ðk k Þ are described bywhere m à is the effective mass. The two E AE ðk k Þ parabolas are shifted relative to the origin " À (k k ¼ 0) by a momentum splitting Ák k ¼ ðm à R Þ=@ 2 . The Rashba effect has been investigated first and foremost for semiconductor heterostructures [2], reaching Rashba parameters of up to 4  10 À11 eV m in InAs-based structures [5]. As for metal surfaces and interfaces, their applications in spintronics are rather conditional and restrained by bulk conductivity of the materials. Nevertheless, metal surfaces remain crucially important model systems for elucidating the physical aspects of the Rashba effect. Spin currents produced by the spin Hall effect in all-metal devices are much larger than in semiconductors [6,7], and very large Rashba effects have been measured for metal surface states which are localized at the outermost atomic layers of the solid-vacuum interface. Discovered by Russian theoretician Tamm in 1932 [8], metal surface states had to wait for their experimental scrutiny until ultrahigh vacuum sample environments became available [9]. They are highly sensitive to adsorbates, and it is hard to conceive an adsorbate that will leave a surface state unaffe...

SmB6 is predicted to be the first member of the intersection of topological insulators and Kondo insulators, strongly correlated materials in which the Fermi level lies in the gap of a many-body resonance that forms by hybridization between localized and itinerant states. While robust, surface-only conductivity at low temperature and the observation of surface states at the expected high symmetry points appear to confirm this prediction, we find both surface states at the (100) surface to be topologically trivial. We find the state to appear Rashba split and explain the prominent state by a surface shift of the many-body resonance. We propose that the latter mechanism, which applies to several crystal terminations, can explain the unusual surface conductivity. While additional, as yet unobserved topological surface states cannot be excluded, our results show that a firm connection between the two material classes is still outstanding.