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Register a new userIn-Plane Orbital Texture Switch at the Dirac Point in the Topological Insulator Bi2Se3
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Topological insulators are novel macroscopic quantum-mechanical phase of matter, which hold promise for realizing some of the most exotic particles in physics as well as application towards spintronics and quantum computation. In all the known topological insulators, strong spin-orbit coupling is critical for the generation of the protected massless surface states. Consequently, a complete description of the Dirac state should include both the spin and orbital (spatial) parts of the wavefunction. For the family of materials with a single Dirac cone, theories and experiments agree qualitatively, showing the topological state has a chiral spin texture that changes handedness across the Dirac point (DP), but they differ quantitatively on how the spin is polarized. Limited existing theoretical ideas predict chiral local orbital angular momentum on the two sides of the DP. However, there have been neither direct measurements nor calculations identifying the global symmetry of the spatial wavefunction. Here we present the first results from angle-resolved photoemission experiment and first-principles calculation that both show, counter to current predictions, the in-plane orbital wavefunctions for the surface states of Bi2Se3 are asymmetric relative to the DP, switching from being tangential to the k-space constant energy surfaces above DP, to being radial to them below the DP. Because the orbital texture switch occurs exactly at the DP this effect should be intrinsic to the topological physics, constituting an essential yet missing aspect in the description of the topological Dirac state. Our results also indicate that the spin texture may be more complex than previously reported, helping to reconcile earlier conflicting spin resolved measurements.
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We study Bi2Se3 by polarization-dependent angle-resolved photoemission spectroscopy (ARPES) and density-functional theory slab calculations. We find that the surface state Dirac fermions are characterized by a layer-dependent entangled spin-orbital texture, which becomes apparent through quantum interference effects. This explains the discrepancy between the spin polarization from spin-resovled ARPES - ranging from 20 to 85% - and the 100% value assumed in phenomenological models. It also suggests a way to probe the intrinsic spin texture of topological insulators, and to continuously manipulate the spin polarization of photoelectrons and photocurrents all the way from 0 to +/-100% by an appropriate choice of photon energy, linear polarization, and angle of incidence.
We study the manipulation of the photoelectron spin-polarization in Bi$_2$Se$_3$ by spin- and angle-resolved photoemission spectroscopy. General rules are established that enable controlling the spin-polarization of photoemitted electrons via light polarization, sample orientation, and photon energy. We demonstrate the $pm$100% reversal of a single component of the measured spin-polarization vector upon the rotation of light polarization, as well as a full three-dimensional manipulation by varying experimental configuration and photon energy. While a material-specific density-functional theory analysis is needed for the quantitative description, a minimal two-atomic-layer model qualitatively accounts for the spin response based on the interplay of optical selection rules, photoelectron interference, and topological surface-state complex structure. It follows that photoelectron spin-polarization control is generically achievable in systems with a layer-dependent, entangled spin-orbital texture.
While some of the most elegant applications of topological insulators, such as quantum anomalous Hall effect, require the preservation of Dirac surface states in the presence of time-reversal symmetry breaking, other phenomena such as spin-charge conversion rather rely on the ability for these surface states to imprint their spin texture on adjacent magnetic layers. In this work, we investigate the spin-momentum locking of the surface states of a wide range of monolayer transition metals (3$d$-TM) deposited on top of Bi$_{2}$Se$_{3}$ topological insulators using first principles calculations. We find an anticorrelation between the magnetic moment of the 3$d$-TM and the magnitude of the spin-momentum locking {em induced} by the Dirac surface states. While the magnetic moment is large in the first half of the 3$d$ series, following Hunds rule, the spin-momentum locking is maximum in the second half of the series. We explain this trend as arising from a compromise between intra-atomic magnetic exchange and covalent bonding between the 3$d$-TM overlayer and the Dirac surface states. As a result, while Cr and Mn overlayers can be used successfully for the observation of quantum anomalous Hall effect or the realization of axion insulators, Co and Ni are substantially more efficient for spin-charge conversion effects, e.g. spin-orbit torque and charge pumping.
Recently discovered materials called three-dimensional topological insulators constitute examples of symmetry protected topological states in the absence of applied magnetic fields and cryogenic temperatures. A hallmark characteristic of these non-magnetic bulk insulators is the protected metallic electronic states confined to the materials surfaces. Electrons in these surface states are spin polarized with their spins governed by their direction of travel (linear momentum), resulting in a helical spin texture in momentum space. Spin- and angle-resolved photoemission spectroscopy (spin-ARPES) has been the only tool capable of directly observing this central feature with simultaneous energy, momentum, and spin sensitivity. By using an innovative photoelectron spectrometer with a high-flux laser-based light source, we discovered another surprising property of these surface electrons which behave like Dirac fermions. We found that the spin polarization of the resulting photoelectrons can be fully manipulated in all three dimensions through selection of the light polarization. These surprising effects are due to the spin-dependent interaction of the helical Dirac fermions with light, which originates from the strong spin-orbit coupling in the material. Our results illustrate unusual scenarios in which the spin polarization of photoelectrons is completely different from the spin state of electrons in the originating initial states. The results also provide the basis for a novel source of highly spin-polarized electrons with tunable polarization in three dimensions.
We characterize the topological insulator Bi$_2$Se$_3$ using time- and angle- resolved photoemission spectroscopy. By employing two-photon photoemission, a complete picture of the unoccupied electronic structure from the Fermi level up to the vacuum level is obtained. We demonstrate that the unoccupied states host a second, Dirac surface state which can be resonantly excited by 1.5 eV photons. We then study the ultrafast relaxation processes following optical excitation. We find that they culminate in a persistent non-equilibrium population of the first Dirac surface state, which is maintained by a meta-stable population of the bulk conduction band. Finally, we perform a temperature-dependent study of the electron-phonon scattering processes in the conduction band, and find the unexpected result that their rates decrease with increasing sample temperature. We develop a model of phonon emission and absorption from a population of electrons, and show that this counter-intuitive trend is the natural consequence of fundamental electron-phonon scattering processes. This analysis serves as an important reminder that the decay rates extracted by time-resolved photoemission are not in general equal to single electron scattering rates, but include contributions from filling and emptying processes from a continuum of states.
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