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.

Ferromagnetic topological insulators exhibit the quantum anomalous Hall effect, which is potentially useful for high‐precision metrology, edge channel spintronics, and topological qubits.  The stable 2+ state of Mn enables intrinsic magnetic topological insulators. MnBi2Te4 is, however, antiferromagnetic with 25 K Néel temperature and is strongly n‐doped. In this work, p‐type MnSb2Te4, previously considered topologically trivial, is shown to be a ferromagnetic topological insulator for a few percent Mn excess. i) Ferromagnetic hysteresis with record Curie temperature of 45–50 K, ii) out‐of‐plane magnetic anisotropy, iii) a 2D Dirac cone with the Dirac point close to the Fermi level, iv) out‐of‐plane spin polarization as revealed by photoelectron spectroscopy, and v) a magnetically induced bandgap closing at the Curie temperature, demonstrated by scanning tunneling spectroscopy (STS), are shown. Moreover, a critical exponent of the magnetization β ≈ 1 is found, indicating the vicinity of a quantum critical point. Ab initio calculations reveal that Mn–Sb site exchange provides the ferromagnetic interlayer coupling and the slight excess of Mn nearly doubles the Curie temperature. Remaining deviations from the ferromagnetic order open the inverted bulk bandgap and render MnSb2Te4 a robust topological insulator and new benchmark for magnetic topological insulators.

Using spin-and angle-resolved spectroscopy and relativistic many-body calculations, we investigate the evolution of the electronic structure of (Bi1−xInx)2Se3 bulk single crystals around the critical point of the trivial to topological insulator quantum-phase transition. By increasing x, we observe how a surface gap opens at the Dirac point of the initially gapless topological surface state of Bi2Se3, leading to the existence of massive fermions. The surface gap monotonically increases for a wide range of x values across the topological and trivial sides of the quantum-phase transition. By means of photon-energy dependent measurements, we demonstrate that the gapped surface state survives the inversion of the bulk bands which occurs at a critical point near x = 0.055. The surface state exhibits a non-zero in-plane spin polarization which decays exponentially with increasing x, and that persists on both the topological and trivial insulator phases. Its out-of-plane spin polarization remains zero demonstrating the absence of a hedgehog spin texture expected from broken time-reversal symmetry. Our calculations reveal qualitative agreement with the experimental results all across the quantum-phase transition upon the systematic variation of the spin-orbit coupling strength. A non-time reversal symmetry breaking mechanism of bulk-mediated scattering processes that increase with decreasing spin-orbit coupling strength is proposed as explanation.

Ultrafast dynamics in three-dimensional topological insulators (TIs) opens new routes for increasing the speed of information transport up to frequencies thousand times faster than in modern electronics. However, up to date, disentangling the exact contributions from bulk and surface transport to the subpicosecond dynamics of these materials remains a difficult challenge. Here, using timeand angle-resolved photoemission, we demonstrate that driving a TI from the bulk-conducting into the bulk-insulating transport regime allows to selectively switch on and off the emergent channels of ultrafast transport between the surface and the bulk. We thus establish that ultrafast transport is one of the main driving mechanisms responsible for the decay of excited electrons in prototypical TIs following laser excitation. We further show how ultrafast transport strongly affects the thermalization and scattering dynamics of the excited states up to high energies above the Fermi level. In particular, we observe how inhibiting the transport channels leads to a thermalization bottleneck that substantially slows down electron-hole recombination via electron-electron scatterings. Our results pave the way for exploiting ultrafast transport to control thermalization time scales in TI-based optoelectronic applications, and expand the capabilities of TIs as intrinsic solar cells.

Topological phases of matter offer exciting possibilities to realize lossless charge and spin information transport on ultrafast time scales. However, this requires detailed knowledge of their nonequilibrium properties. Here, we employ time-, spin- and angle-resolved photoemission to investigate the ultrafast response of the Sb(111) spin-polarized surface state to femtosecond-laser excitation. The surface state exhibits a giant mass enhancement which is observed as a kink structure in its energy-momentum dispersion above the Fermi level. The kink structure, originating from the direct coupling of the surface state to the bulk continuum, is characterized by an abrupt change in the group velocity by ~70%, in agreement with our GW-based band structure calculations. Our observation of this connectivity in the transiently occupied band structure enables the unambiguous experimental verification of the topological nature of the surface state. The influence of bulk-surface coupling is further confirmed by our measurements of the electron dynamics, which show that bulk and surface states behave as a single thermalizing electronic population with distinct contributions from low-k electron-electron and high-k electron-phonon scatterings. These findings are important for future applications of topological semimetals and their excitations in ultrafast spintronics.

The Dirac point of a topological surface state (TSS) is protected against gapping by time-reversal symmetry. Conventional wisdom stipulates, therefore, that only through magnetisation may a TSS become gapped. However, non-magnetic gaps have now been demonstrated in Bi2Se3 systems doped with Mn or In, explained by hybridisation of the Dirac cone with induced impurity resonances. Recent photoemission experiments suggest that an analogous mechanism applies even when Bi2Se3 is surface dosed with Au. Here, we perform a systematic spin- and angle-resolved photoemission study of Au-dosed Bi2Se3. Although there are experimental conditions wherein the TSS appears gapped due to unfavourable photoemission matrix elements, our photon-energy-dependent spectra unambiguously demonstrate the robustness of the Dirac cone against high Au coverage. We further show how the spin textures of the TSS and its accompanying surface resonances remain qualitatively unchanged following Au deposition, and discuss the mechanism underlying the suppression of the spectral weight.

A large Rashba effect is essential for future applications in spintronics. Particularly attractive is understanding and controlling nonequilibrium properties of ferroelectric Rashba semiconductors. Here, time‐ and angle‐resolved photoemission is utilized to access the ultrafast dynamics of bulk and surface transient Rashba states after femtosecond optical excitation of GeTe. A complex thermalization pathway is observed, wherein three different timescales can be clearly distinguished: intraband thermalization, interband equilibration, and electronic cooling. These dynamics exhibit an unconventional temperature dependence: while the cooling phase speeds up with increasing sample temperature, the opposite happens for interband thermalization. It is demonstrated how, due to the Rashba effect, an interdependence of these timescales on the relative strength of both electron–electron and electron–phonon interactions is responsible for the counterintuitive temperature dependence, with spin‐selection constrained interband electron–electron scatterings found both to dominate dynamics away from the Fermi level, and to weaken with increasing temperature. These findings are supported by theoretical calculations within the Boltzmann approach explicitly showing the opposite behavior of all relevant electron–electron and electron–phonon scattering channels with temperature, thus confirming the microscopic mechanism of the experimental findings. The present results are important for future applications of ferroelectric Rashba semiconductors and their excitations in ultrafast spintronics.

We show that, although the equilibrium band dispersion of the Shockley-type surface state of two-dimensional Au(111) quantum films grown on W(110) does not deviate from the expected free-electron-like behavior, its nonequilibrium energy-momentum dispersion probed by time-and angle-resolved photoemission exhibits a remarkable kink above the Fermi level due to a significant enhancement of the effective mass. The kink is pronounced for certain thicknesses of the Au quantum well and vanishes in the very thin limit. We identify the kink as induced by the coupling between the Au(111) surface state and emergent quantum-well states which probe directly the buried gold-tungsten interface. The signatures of the coupling are further revealed by our time-resolved measurements which show that surface state and quantum-well states thermalize together behaving as dynamically locked electron populations. In particular, relaxation of hot carriers following laser excitation is similar for both surface state and quantum-well states and much slower than expected for a bulk metallic system. The influence of quantum confinement on the interplay between elementary scattering processes of the electrons at the surface and ultrafast carrier transport in the direction perpendicular to the surface is shown to be the reason for the slow electron dynamics.