L. Patthey

A tunable topological insulator in the spin helical Dirac transport regime

Helical Dirac fermions—charge carriers that behave as massless relativistic particles with an intrinsic angular momentum (spin) locked to its translational momentum—are proposed to be the key to realizing fundamentally new phenomena in condensed matter physics. Prominent examples include the anomalous quantization of magneto-electric coupling, half-fermion states that are their own antiparticle, and charge fractionalization in a Bose–Einstein condensate, all of which are not possible with conventional Dirac fermions of the graphene variety. Helical Dirac fermions have so far remained elusive owing to the lack of necessary spin-sensitive measurements and because such fermions are forbidden to exist in conventional materials harbouring relativistic electrons, such as graphene or bismuth. It has recently been proposed that helical Dirac fermions may exist at the edges of certain types of topologically ordered insulators—materials with a bulk insulating gap of spin–orbit origin and surface states protected against scattering by time-reversal symmetry—and that their peculiar properties may be accessed provided the insulator is tuned into the so-called topological transport regime. However, helical Dirac fermions have not been observed in existing topological insulators. Here we report the realization and characterization of a tunable topological insulator in a bismuth-based class of material by combining spin-imaging and momentum-resolved spectroscopies, bulk charge compensation, Hall transport measurements and surface quantum control. Our results reveal a spin-momentum locked Dirac cone carrying a non-trivial Berry’s phase that is nearly 100 per cent spin-polarized, which exhibits a tunable topological fermion density in the vicinity of the Kramers point and can be driven to the long-sought topological spin transport regime. The observed topological nodal state is shown to be protected even up to 300 K. Our demonstration of room-temperature topological order and non-trivial spin-texture in stoichiometric Bi2Se3.Mx (Mx indicates surface doping or gating control) paves the way for future graphene-like studies of topological insulators, and applications of the observed spin-polarized edge channels in spintronic and computing technologies possibly at room temperature.Princeton University, Princeton, NJ 08544, USA Department of Physics, Shanghai Jiao Tong University, Shanghai 200030, China Swiss Light Source, Paul Scherrer Institute, CH-5232, Villigen, Switzerland Physik-Institut, Universität Zürich-Irchel, 8057 Zürich, Switzerland Advanced Light Source, Lawrence Berkeley Laboratory, Berkeley, CA 94720, USA Department of Physics, Northeastern University, Boston, MA 02115, USA Department of Chemistry, Princeton University, Princeton, NJ 08544, USA Princeton Center for Complex Materials, Princeton University, Princeton NJ 08544, USA

Experimental evidence for sub-3-fs charge transfer from an aromatic adsorbate to a semiconductor

The ultrafast timescale of electron transfer processes is crucial to their role in many biological systems and technological devices. In dye-sensitized solar cells, the electron transfer from photo-excited dye molecules to nanostructured semiconductor substrates needs to be sufficiently fast to compete effectively against loss processes and thus achieve high solar energy conversion efficiencies. Time-resolved laser techniques indicate an upper limit of 20 to 100 femtoseconds for the time needed to inject an electron from a dye into a semiconductor, which corresponds to the timescale on which competing processes such as charge redistribution and intramolecular thermalization of excited states occur. Here we use resonant photoemission spectroscopy, which has previously been used to monitor electron transfer in simple systems with an order-of-magnitude improvement in time resolution, to show that electron transfer from an aromatic adsorbate to a TiO2 semiconductor surface can occur in less than 3 fs. These results directly confirm that electronic coupling of the aromatic molecule to its substrate is sufficiently strong to suppress competing processes.

Electronic structure of atomically precise graphene nanoribbons.

Some of the most intriguing properties of graphene are predicted for specifically designed nanostructures such as nanoribbons. Functionalities far beyond those known from extended graphene systems include electronic band gap variations related to quantum confinement and edge effects, as well as localized spin-polarized edge states for specific edge geometries. The inability to produce graphene nanostructures with the needed precision, however, has so far hampered the verification of the predicted electronic properties. Here, we report on the electronic band gap and dispersion of the occupied electronic bands of atomically precise graphene nanoribbons fabricated via on-surface synthesis. Angle-resolved photoelectron spectroscopy and scanning tunneling spectroscopy data from armchair graphene nanoribbons of width N = 7 supported on Au(111) reveal a band gap of 2.3 eV, an effective mass of 0.21 m(0) at the top of the valence band, and an energy-dependent charge carrier velocity reaching 8.2 × 10(5) m/s in the linear part of the valence band. These results are in quantitative agreement with theoretical predictions that include image charge corrections accounting for screening by the metal substrate and confirm the importance of electron-electron interactions in graphene nanoribbons.

Adsorption of Bi-Isonicotinic Acid on Rutile TiO2 (110)

Bi-isonicotinic acid ~2,28-bipyridine–4,48-dicarboxylic acid! is the ligand of several organometallic dyes, used in photoelectrochemical applications. Therefore the atomic scale understanding of the bonding of this molecule to rutile TiO2(110) should give insight into the crucial dye–surface interaction. High resolution x-ray photoelectron spectroscopy ~XPS!, near edge x-ray absorption fine structure ~NEXAFS!, and periodic intermediate neglect of differential overlap ~INDO! calculations were carried out on submonolayer bi-isonicotinic acid rutile TiO2(110). Data from multilayers is also presented to support the submonolayer results. For a multilayer, XPS shows that the carboxyl groups remain in the ~pristine! protonated form, and NEXAFS show that the molecular plane is tilted by 57° with respect to the surface normal. For the submonolayer, the molecule bonds to the rutile TiO2(110) surface via both deprotonated carboxyl groups, with a tilt angle of 25°, and additionally an azimuthal orientation of 44° with respect to the @001# crystallographic direction. The adsorbant system was also investigated by quantum mechanical calculations using a periodic INDO model. The most stable theoretical adsorption geometry involves a twist around the molecular axis, such that the pyridine rings are tilted in opposite directions. Both oxygen atoms of each carboxyl group are bonded to five-fold coordinated Ti atoms ~2M-bidentate!, in excellent agreement with the experimental results.

SAXES, a high resolution spectrometer for resonant x-ray emission in the 400-1600 eV energy range

We present a 5m long spectrometer for soft x rays to be used at a synchrotron radiation beamline for resonant x-ray emission spectroscopy and resonant inelastic x-ray scattering in the 400–1600eV energy range. It is based on a variable line spacing spherical grating (average groove density of 3200mm−1, R=58.55m) and a charge coupled device two dimensional detector. With an x-ray spot on the sample of 10μm, the targeted resolving power is higher than 10 000 at all energies below 1100eV and better than 7000 at 1500eV. The off-line tests made with Al and MgKα1,2 fluorescence emissions indicate that the spectrometer can actually work at 12 000 and 17 000 resolving power at the L3 edges of Cu (930eV) and of Ti (470eV), respectively. SAXES (superadvanced x-ray emission spectrometer) is mounted on a rotating platform allowing to vary the scattering angle from 25° to 130°. The spectrometer will be operational at the ADRESS (advanced resonant spectroscopies) beamline of the Swiss Light Source from 2007.

Spin-orbital separation in the quasi-one-dimensional Mott insulator Sr2CuO3

When viewed as an elementary particle, the electron has spin and charge. When binding to the atomic nucleus, it also acquires an angular momentum quantum number corresponding to the quantized atomic orbital it occupies. Even if electrons in solids form bands and delocalize from the nuclei, in Mott insulators they retain their three fundamental quantum numbers: spin, charge and orbital. The hallmark of one-dimensional physics is a breaking up of the elementary electron into its separate degrees of freedom. The separation of the electron into independent quasi-particles that carry either spin (spinons) or charge (holons) was first observed fifteen years ago. Here we report observation of the separation of the orbital degree of freedom (orbiton) using resonant inelastic X-ray scattering on the one-dimensional Mott insulator Sr2CuO3. We resolve an orbiton separating itself from spinons and propagating through the lattice as a distinct quasi-particle with a substantial dispersion in energy over momentum, of about 0.2 electronvolts, over nearly one Brillouin zone.

Evidence for an excitonic insulator phase in 1T-TiSe2.

We present a new high-resolution angle-resolved photoemission study of 1T-TiSe2 in both its room-temperature, normal phase and its low-temperature, charge-density wave phase. At low temperature the photoemission spectra are strongly modified, with large band renormalizations at high-symmetry points of the Brillouin zone and a very large transfer of spectral weight to backfolded bands. A calculation of the theoretical spectral function for an excitonic insulator phase reproduces the experimental features with very good agreement. This gives strong evidence in favor of the excitonic insulator scenario as a driving force for the charge-density wave transition in 1T-TiSe2.

Large-Amplitude Spin Dynamics Driven by a THz Pulse in Resonance with an Electromagnon

Ultrafast Manipulation Multiferroic materials commonly show both magnetism and ferroelectricity, such that the electric field can be used to manipulate the magnetic order, and vice versa. Kubacka et al. (p. 1333, published online 6 March) used a strong terahertz electromagnetic pulse in resonance with an electromagnon—an excitation based on both electric and magnetic ordering—to control the spin dynamics of the multiferroic TbMnO3 on a sub-picosecond time scale and induce the rotation of the spin-cycloid plane of the material. The electric field of an electromagnetic pulse exerts ultrafast control on the spin dynamics of the multiferroic TbMnO3. Multiferroics have attracted strong interest for potential applications where electric fields control magnetic order. The ultimate speed of control via magnetoelectric coupling, however, remains largely unexplored. Here, we report an experiment in which we drove spin dynamics in multiferroic TbMnO3 with an intense few-cycle terahertz (THz) light pulse tuned to resonance with an electromagnon, an electric-dipole active spin excitation. We observed the resulting spin motion using time-resolved resonant soft x-ray diffraction. Our results show that it is possible to directly manipulate atomic-scale magnetic structures with the electric field of light on a sub-picosecond time scale.

Emergent quantum confinement at topological insulator surfaces

Bismuth-chalchogenides are model examples of three-dimensional topological insulators. Their ideal bulk-truncated surface hosts a single spin-helical surface state, which is the simplest possible surface electronic structure allowed by their non-trivial Z(2) topology. However, real surfaces of such compounds, even if kept in ultra-high vacuum, rapidly develop a much more complex electronic structure whose origin and properties have proved controversial. Here we demonstrate that a conceptually simple model, implementing a semiconductor-like band bending in a parameter-free tight-binding supercell calculation, can quantitatively explain the entire measured hierarchy of electronic states. In combination with circular dichroism in angle-resolved photoemission experiments, we further uncover a rich three-dimensional spin texture of this surface electronic system, resulting from the non-trivial topology of the bulk band structure. Moreover, our study sheds new light on the surface-bulk connectivity in topological insulators, and reveals how this is modified by quantum confinement.

Atom-specific spin mapping and buried topological states in a homologous series of topological insulators

A topological insulator is a state of quantum matter that, while being an insulator in the bulk, hosts topologically protected electronic states at the surface. These states open the opportunity to realize a number of new applications in spintronics and quantum computing. To take advantage of their peculiar properties, topological insulators should be tuned in such a way that ideal and isolated Dirac cones are located within the topological transport regime without any scattering channels. Here we report ab-initio calculations, spin-resolved photoemission and scanning tunnelling microscopy experiments that demonstrate that the conducting states can effectively tuned within the concept of a homologous series that is formed by the binary chalcogenides (Bi(2)Te(3), Bi(2)Se(3) and Sb(2)Te(3)), with the addition of a third element of the group IV.