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How quanta of energy and charge are transported on both atomic spatial and ultrafast time scales is at the heart of modern technology. Recent progress in ultrafast spectroscopy has allowed us to directly study the dynamical response of an electronic system to interaction with an electromagnetic field. Here, we present energy-dependent photoemission delays from the noble metal surfaces Ag(111) and Au(111). An interferometric technique based on attosecond pulse trains is applied simultaneously in a gas phase and a solid state target to derive surface-specific photoemission delays. Experimental delays on the order of 100 as are in the same time range as those obtained from simulations. The strong variation of measured delays with excitation energy in Ag(111), which cannot be consistently explained invoking solely electron transport or initial state localization as supposed in previous work, indicates that final state effects play a key role in photoemission from solids.

We present time-resolved photoemission experiments from a peculiar bismuth surface, Bi(114). The strong one-dimensional character of this surface is reflected in the Fermi surface, which consists of spin-polarized straight lines. Our results show that the depletion of the surface state and the population of the bulk conduction band after the initial optical excitation persist for very long times. The disequilibrium within the hot electron gas along with strong electron-phonon coupling cause a displacive excitation of coherent phonons, which in turn are reflected in coherent modulations of the electronic states. Beside the well-known A1g bulk phonon mode at 2.76 THz the time-resolved photoelectron spectra reveal a second mode at 0.72 THz which can be attributed to an optical surface phonon mode along the atomic rows of the Bi(114) surface., Comment: 5 pages, 4 figures

The surface of topological insulators is proposed as a promising platform for spintronics and quantum information applications. In particular, when time- reversal symmetry is broken, topological surface states are expected to exhibit a wide range of exotic spin phenomena for potential implementation in electronics. Such devices need to be fabricated using nanoscale artificial thin films. It is of critical importance to study the spin behavior of artificial topological MBE thin films associated with magnetic dopants, and with regards to quantum size effects related to surface-to-surface tunneling as well as experimentally isolate time-reversal breaking from non-intrinsic surface electronic gaps. Here we present observation of the first (and thorough) study of magnetically induced spin reorientation phenomena on the surface of a topological insulator. Our results reveal dramatic rearrangements of the spin configuration upon magnetic doping contrasted with chemically similar nonmagnetic doping as well as with quantum tunneling phenomena in ultra-thin high quality MBE films. While we observe that the spin rearrangement induced by quantum tunneling occurs in a time-reversal invariant fashion, we present critical and systematic observation of an out-of-plane spin texture evolution correlated with magnetic interactions, which breaks time-reversal symmetry, demonstrating microscopic TRB at a Kramers' point on the surface., Comment: 12 pages, 3 Figures, Related results at http://online.kitp.ucsb.edu/online/topomat11/hasan/oh/01.html

We perform spin-resolved and spin-integrated angle-resolved photoemission spectroscopy measurements on a series of compositions in the BiTl(S1-xSex)2 system, focusing on x-values in the vicinity of the critical point for the topological phase transition (the band inversion composition). We observe quasi two dimensional (2D) states on the outer boundary of the bulk electronic bands in the trivial side (non-inverted regime) of the transition. Systematic spin-sensitive measurements reveal that the observed 2D states are spin-momentum locked, whose spin texture resembles the helical spin texture on the surface of a topological insulator. These anomalous states are observed to be only prominent near the critical point, thus are possibly related to strong precursor states of topological phase transition near the relaxed surface., Comment: 5 pages, 4 figures

The recently discovered three dimensional or bulk topological insulators are expected to exhibit exotic quantum phenomena. It is believed that a trivial insulator can be twisted into a topological state by modulating the spin-orbit interaction or the crystal lattice via odd number of band inversions, driving the system through a topological quantum phase transition. By directly measuring the topological invariants (for the method to directly measure Fu-Kane {$\nu_0$}, see Hsieh \textit{et.al.,} Science 323, 919 (2009) at http://www.sciencemag.org/content/323/5916/919.abstract) we report the observation of a phase transition in a tunable spin-orbit system BiTl(S{1-d}Se{d})2 (which is an analog of the most studied topological insulator Bi2Se3, see Xia \textit{et.al.,} Nature Phys. 5, 398 (2009) at http://www.nature.com/nphys/journal/v5/n6/full/nphys1294.html and Spin-Momentum locking at http://www.nature.com/nature/journal/v460/n7259/full/nature08234.html) where the topological insulator state formation is visualized for the first time. In the topological state, vortex-like polarization states are observed to exhibit 3D vectorial textures, which collectively feature a chirality transition of its topological spin-textures as the spin-momentum locked (Z2 topologically ordered) electrons on the surface go through the zero carrier density point. Such phase transition and texture chirality inversion can be the physical basis for observing \textit{fractional charge} (e/2) and other related fractional topological phenomena., Comment: 13 pages, 4 Figures, Accepted for publication in Science (published at ScienceExpress on 31 March, 2011)

We report high-resolution spin-resolved photoemission spectroscopy (Spin-ARPES) measurements on the parent compound Sb of the first discovered 3D topological insulator Bi{1-x}Sb{x} [D. Hsieh et al., Nature 452, 970 (2008) Submitted 2007]. By modulating the incident photon energy, we are able to map both the bulk and (111) surface band structure, from which we directly demonstrate that the surface bands are spin polarized by the spin-orbit interaction and connect the bulk valence and conduction bands in a topologically non-trivial way. A unique asymmetric Dirac surface state gives rise to a $k$-splitting of its spin polarized electronic channels. These results complement our previously published works on this materials class and re-confirm our discovery of first bulk (3D) topological insulator - topological order in bulk solids. [Invited article for NJP-IOP Focus issue on "Topological Insulators"], Comment: Invited article for NJP-IOP Focus issue on "Topological Insulators", Experimental discovery of 3D topological insulators (topological order in bulk solids) reported at KITP (2007) Conference Proceeding at http://online.itp.ucsb.edu/online/motterials07/hasan/ (2007)

We report a Rashba spin splitting of a two-dimensional electron gas in the topological insulator Bi$_2$Se$_3$ from angle-resolved photoemission spectroscopy. We further demonstrate its electrostatic control, and show that spin splittings can be achieved which are at least an order-of-magnitude larger than in other semiconductors. Together these results show promise for the miniaturization of spintronic devices to the nanoscale and their operation at room temperature., Comment: 5 pages, 4 figures. Substantially revised

The development of spin-based applications of topological insulators requires the knowledge and understanding of spin texture configuration maps as they change via gating in the vicinity of an isolated Dirac node. An isolated (graphene-like) Dirac node, however, does not exist in Bi2Te3. While the isolation of surface states via transport channels has been promisingly achieved in Bi2Te3, it is not known how spin textures modulate while gating the surface. Another drawback of Bi2Te3 is that it features multiple band crossings while chemical potential is placed near the Dirac node (at least 3 not one as in Bi2Se3 and many other topological insulators) and its buried Dirac point is not experimentally accessible for the next generation of experiments which require tuning the chemical potential near an isolated (graphene-like) Dirac node. Here, we image the spin texture of Bi2Te3 and suggest a simple modification to realize a much sought out isolated Dirac node regime critical for almost all potential applications (of topological nature) of Bi2Te3. Finally, we demonstrate carrier control in magnetically and nonmagnetically doped Bi2Te3 essential for realizing giant magneto-optical effects and dissipationless spin current devices involving a Bi2Te3-based platform., Comment: 5 pages, 4 Figures

A topological insulator is characterized by spin-momentum locking on its boundary. The spin momentum locking on the surface of a three dimensional topological insulator leads to the existence of a non-trivial Berry's phase which leads to exotic transport phenomena on topological surfaces. Using spin-sensitive probes (Mott polarimetry), we observe the spin-momentum coupling and uncover the chiral nature of surface electrons in TlBiSe2. We demonstrate that the surface electrons in TlBiSe2 collectively carry a quantum Berry's phase of $\pi$ and a definite chirality ($\eta$ = -1, left-handed) associated with its spin-texture or vortex-structure on the Fermi surface on both the top and the bottom surfaces. Our experimental results for the first time not only prove the existence of Z2 topological-order in the bulk but also reveal the existence of helical quasiparticle modes on the topological surface. Spin-texture calculations would be reported elsewhere., Comment: 4 pages, 2 Figures, Results are incorporated into the Supplementary Info (SOM) Section of Science 332, 560 (2011)

Both the theoretical and experimental discovery of single-Dirac-cone topological-insulator-class was reported at arXiv:0812.2078 (2008) [Y. Xia et.al., Nature Physics 5, 398-402 (2009) http://www.nature.com/nphys/journal/v5/n6/full/nphys1294.html]. Here we report the first observation of Spin-Momentum Helical Locking and Spin-Vortex structures in Bi2Se3 and Bi2Te3, demonstrate the existence of Topological-Order at 300K and report a material realization of topological-transport-regime for helical Dirac fermions. Our results reveal a one-to-one spin-momentum locked Dirac structure in Bi2Se3 and Bi2Te3 that is nearly 100% 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-transport-regime. The observed topological nodal Dirac ground state is found to be protected even up to room temperature (300 K). Our results pave the way for future transport based studies of topological insulators, and possible room temperature applications of protected spin-polarized edge channels we observe with spin-ARPES in spintronic technology. All of these new results are made possible due to the Spin-resolved-ARPES (Mott polarimetric) technique [http://www.nature.com/nature/journal/v460/n7259/full/nature08234.html ] ., Comment: 17 pages, 4 Figures, Published nature-Online in July-2009, Submitted to NATURE in April-2009

The interaction of atomic hydrogen with a single layer of hexagonal boron nitride on rhodium leads to a removal of the h-BN surface corrugation. The process is reversible as the hydrogen may be expelled by annealing to about 500 K whereupon the texture on the nanometer scale is restored. This effect is traced back to hydrogen intercalation. It is expected to have implications for applications, like the storage of hydrogen, the peeling of sp2-hybridized layers from solid substrates or the control of the wetting angle, to name a few., Comment: 4 pages and 4 figures

A topologically ordered material is characterized by a rare quantum organization of electrons that evades the conventional spontaneously broken symmetry based classification of condensed matter. Exotic spin transport phenomena such as the dissipationless quantum spin Hall effect have been speculated to originate from a novel topological order whose identification requires a spin sensitive measurement. Using Spin-resolved-ARPES, we probe the spin degrees of freedom and demonstrate that topological quantum numbers are uniquely determined from spin-texture Berry Phase imaging measurements. Applying this method to pure antimony (Sb) and Bi-Sb, we identify the origin of its novel Topological Order and the negative value of the mirror Chern number. These results taken together constitute the first observation of surface electrons collectively carrying a topological Berry's phase and definite mirror Chern chirality in pure Antimony (Sb) which are the key electronic properties for realizing topological quantum computing via the interface Majorana fermion framework. This paper contains the details of the above mentioned previously reported (Science \textbf{323}, 919 (2009)) results., Comment: 6 Figures, 10 Pages, RevTex Format, Detailed version of Hsieh et.al., SCIENCE 323, 919 (2009)

We show that the strongly spin-orbit coupled materials Bi2Te3 and Sb2Te3 (first non-Bi topological insulator) and their derivatives belong to the Z2 (Time-Reversal-Protected, elastic backscattering suppressed) topological-insulator class. Using a combination of first-principles theoretical calculations and photoemission spectroscopy, we directly show that Bi2Te3 is a large spin-orbit-induced indirect bulk band gap (about 150 meV) semiconductor whose surface is characterized by a single topological spin-Dirac cone. The electronic structure of self-doped Sb2Te3 exhibits similar Z2 topological properties. We demonstrate that the dynamics of surface spin-only Dirac fermions can be controlled through systematic Mn doping, making these materials classes potentially suitable for exploring novel topological physics. We emphasize (theoretically and experimentally) that the Dirac node is well within the bulk-gap and not degenerate with the bulk valence band., Comment: 5 Pages, 4 Figures, Accepted for publication in Physical Review Letters (submitted, June 2009)

Electron systems that possess light-like dispersion relations or the conical Dirac spectrum, such as graphene and bismuth, have recently been shown to harbor unusual collective states in high magnetic fields. Such states are possible because their light-like electrons come in spin pairs that are chiral,which means that their direction of propagation is tied to a quantity called pseudospin that describes their location in the crystal lattice. An emerging direction in quantum materials research is the manipulation of atomic spin-orbit coupling to simulate the effect of a spin dependent magnetic field,in attempt to realize novel spin phases of matter. This effect has been proposed to realize systems consisting of unpaired Dirac cones that are helical, meaning their direction of propagation is tied to the electron spin itself, which are forbidden to exist in graphene or bismuth. The experimental existence of topological order can not be determined without spin-resolved measurements. Here we report a spin-and angle-resolved photoemission study of the hexagonal surface of the Bi2Te3 and Bi{2-x}MnxTe3 series, which is found to exhibit a single helical Dirac cone that is fully spin-polarized. Our observations of a gap in the bulk spin-degenerate band and a spin-resolved surface Dirac node close to the chemical potential show that the low energy dynamics of Bi2Te3 is dominated by the unpaired spin-helical Dirac modes. Our spin-texture measurements prove the existence of a rare topological phase in this materials class for the first time, and suggest its suitability for novel 2D Dirac spin device applications beyond the chiral variety or traditional graphene., Comment: 13 pages, 4 figures

A topologically ordered material is characterized by a rare quantum organization of electrons that evades the conventional spontaneously broken symmetry based classification of condensed matter. Exotic spin transport phenomena such as the dissipationless quantum spin Hall effect have been speculated to originate from a novel topological order whose identification requires a spin sensitive measurement, which does not exist to this date in any system (neither in Hg(Cd)Te quantum wells nor in the topological insulator BiSb). Using Mott polarimetry, we probe the spin degrees of freedom of these quantum spin Hall states and demonstrate that topological quantum numbers are uniquely determined from spin texture imaging measurements. Applying this method to the Bi{1-x}Sb{x} series, we identify the origin of its novel order and unusual chiral properties. These results taken together constitute the first observation of surface electrons collectively carrying a geometrical quantum (Berry's) phase and definite chirality (mirror Chern number, n_M =-1), which are the key electronic properties for realizing topological computing bits with intrinsic spin Hall-like topological phenomena. Our spin-resolved results not only provides the first clear proof of a topological insulating state in nature but also demonstrate the utility of spin-resolved ARPES technique in measuring the quantum spin Hall phases of matter., Comment: 15 pages, 3 figures, first Submitted to SCIENCE on July-22, 2008

Single sheets of hexagonal boron nitride on transition metals provide a model system for single layer dielectrics. The progress in the understanding of h-BN layers on transition metals of the last 10 years are shortly reviewed. Particular emphasis lies on the boron nitride nanomesh on Rh(111), which is a corrugated single sheet of h-BN, where the corrugation imposes strong lateral electric fields. Fermi surface maps of h-BN/Rh(111) and Rh(111) are compared. A h-BN layer on Rh(111) introduces no new bands at the Fermi energy, which is expected for an insulator. The lateral electric fields of h-BN nanomesh violate the conservation law for parallel momentum in photoemission and smear out the momentum distribution curves on the Fermi surface., Comment: 14 pages, 6 figures, 1 table, 1 equation, Accepted for publication in the Special Surface Science issue in honor of Gerhard Ertl's Nobel Prize

The electric field governing the dynamics of space charge produced by high intensity femtosecond laser pulses focused on a copper surface is investigated by time-resolved low-energy-electron-scattering. The pump-probe experiment has a measured temporal resolution of better than 35 ps at 55 eV probe electron energy. The probe electron acceleration due to space charge is reproduced within a 3-dimensional non-relativistic model, which determines an effective number of electrons in the space charge electron cloud and its initial diameter. Comparison of the simulations with the experiments indicates a Coulomb explosion, which is consistent with transients in the order of 1 ns, the terminal kinetic energy of the cloud and the thermoemission currents predicted by the Richardson-Dushman formula., Comment: 10 pages, 4 figures

One monolayer of C60 on one monolayer of hexagonal boron nitride on nickel is investigated by photoemission. Between 150 and 250 K the work function decreases and the binding energy of the highest occupied molecular orbital (HOMO) increases by approx. 100 meV. In parallel, the occupancy of the, in the cold state almost empty, lowest unoccupied molecular orbital (LUMO) changes by 0.4 electrons. This charge redistribution is triggered by onset of molecular rocking motion, i.e. by orientation dependent tunneling between the LUMO of C60 and the substrate. The magnitude of the charge transfer is large and cannot be explained within a single particle picture. It is proposed to involve electron-phonon coupling where C60- polaron formation leads to electron self-trapping., Comment: 15 pages, 4 figures