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.

Atomically Precise Lateral Modulation of a Two-Dimensional Electron Liquid in Anatase TiO2 Thin Films.

Engineering the electronic band structure of two-dimensional electron liquids (2DELs) confined at the surface or interface of transition metal oxides is key to unlocking their full potential. Here we describe a new approach to tailoring the electronic structure of an oxide surface 2DEL demonstrating the lateral modulation of electronic states with atomic scale precision on an unprecedented length scale comparable to the Fermi wavelength. To this end, we use pulsed laser deposition to grow anatase TiO2 films terminated by a (1 × 4) in-plane surface reconstruction. Employing photostimulated chemical surface doping we induce 2DELs with tunable carrier densities that are confined within a few TiO2 layers below the surface. Subsequent in situ angle-resolved photoemission experiments demonstrate that the (1 × 4) surface reconstruction provides a periodic lateral perturbation of the electron liquid. This causes strong backfolding of the electronic bands, opening of unidirectional gaps and a saddle point singularity in the density of states near the chemical potential.

Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr2IrO4.

Measuring how the magnetic correlations evolve in doped Mott insulators has greatly improved our understanding of the pseudogap, non-Fermi liquids and high-temperature superconductivity. Recently, photo-excitation has been used to induce similarly exotic states transiently. However, the lack of available probes of magnetic correlations in the time domain hinders our understanding of these photo-induced states and how they could be controlled. Here, we implement magnetic resonant inelastic X-ray scattering at a free-electron laser to directly determine the magnetic dynamics after photo-doping the Mott insulator Sr2IrO4. We find that the non-equilibrium state, 2 ps after the excitation, exhibits strongly suppressed long-range magnetic order, but hosts photo-carriers that induce strong, non-thermal magnetic correlations. These two-dimensional (2D) in-plane Néel correlations recover within a few picoseconds, whereas the three-dimensional (3D) long-range magnetic order restores on a fluence-dependent timescale of a few hundred picoseconds. The marked difference in these two timescales implies that the dimensionality of magnetic correlations is vital for our understanding of ultrafast magnetic dynamics.

NaFe_{0.56}Cu_{0.44}As: A Pnictide Insulating Phase Induced by On-Site Coulomb Interaction.

In the studies of iron pnictides, a key question is whether their bad-metal state from which the superconductivity emerges lies in close proximity with a magnetically ordered insulating phase. Recently, it was found that at low temperatures, the heavily Cu-doped NaFe_{1-x}Cu_{x}As (x>0.3) iron pnictide is an insulator with long-range antiferromagnetic order, similar to the parent compound of cuprates but distinct from all other iron pnictides. Using angle-resolved photoemission spectroscopy, we determined the momentum-resolved electronic structure of NaFe_{1-x}Cu_{x}As (x=0.44) and identified that its ground state is a narrow-gap insulator. Combining the experimental results with density functional theory (DFT) and DFT+U calculations, our analysis reveals that the on-site Coulombic (Hubbard) and Hund's coupling energies play crucial roles in the formation of the band gap about the chemical potential. We propose that at finite temperatures, charge carriers are thermally excited from the Cu-As-like valence band into the conduction band, which is of Fe 3d-like character. With increasing temperature, the number of electrons in the conduction band becomes larger and the hopping energy between Fe sites increases, and finally the long-range antiferromagnetic order is destroyed at T>T_{N}. Our study provides a basis for investigating the evolution of the electronic structure of a Mott insulator transforming into a bad metallic phase and eventually forming a superconducting state in iron pnictides.

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 Bi(2)Se(3).M(x) (M(x) 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.

Soft-X-ray ARPES facility at the ADRESS beamline of the SLS: concepts, technical realisation and scientific applications.

Soft-X-ray angle-resolved photoelectron spectroscopy (ARPES) with photon energies around 1 keV combines the momentum space resolution with increasing probing depth. The concepts and technical realisation of the new soft-X-ray ARPES endstation at the ADRESS beamline of SLS are described. The experimental geometry of the endstation is characterized by grazing X-ray incidence on the sample to increase the photoyield and vertical orientation of the measurement plane. The vacuum chambers adopt a radial layout allowing most efficient sample transfer. High accuracy of the angular resolution is ensured by alignment strategies focused on precise matching of the X-ray beam and optical axis of the analyzer. The high photon flux of up to 10(13) photons s(-1) (0.01% bandwidth)(-1) delivered by the beamline combined with the optimized experimental geometry break through the dramatic loss of the valence band photoexcitation cross section at soft-X-ray energies. ARPES images with energy resolution up to a few tens of meV are typically acquired on the time scale of minutes. A few application examples illustrate the power of our advanced soft-X-ray ARPES instrumentation to explore the electronic structure of bulk crystals with resolution in three-dimensional momentum, access buried heterostructures and study elemental composition of the valence states using resonant excitation.

High-precision x-ray FEL pulse arrival time measurements at SACLA by a THz streak camera with Xe clusters.

The accurate measurement of the arrival time of a hard X-ray free electron laser (FEL) pulse with respect to a laser is of utmost importance for pump-probe experiments proposed or carried out at FEL facilities around the world. This manuscript presents the latest device to meet this challenge, a THz streak camera using Xe gas clusters, capable of pulse arrival time measurements with an estimated accuracy of several femtoseconds. An experiment performed at SACLA demonstrates the performance of the device at photon energies between 5 and 10 keV with variable photon beam parameters.

Mixed dimensionality of confined conducting electrons in the surface region of SrTiO3.

Using angle-resolved photoemission spectroscopy, we show that the recently discovered surface state on SrTiO(3) consists of nondegenerate t(2g) states with different dimensional characters. While the d(xy) bands have quasi-2D dispersions with weak k(z) dependence, the lifted d(xz)/d(yz) bands show 3D dispersions that differ significantly from bulk expectations and signal that electrons associated with those orbitals permeate the near-surface region. Like their more 2D counterparts, the size and character of the d(xz)/d(yz) Fermi surface components are essentially the same for different sample preparations. Irradiating SrTiO(3) in ultrahigh vacuum is one method observed so far to induce the "universal" surface metallic state. We reveal that during this process, changes in the oxygen valence band spectral weight that coincide with the emergence of surface conductivity are disproportionate to any change in the total intensity of the O 1s core level spectrum. This signifies that the formation of the metallic surface goes beyond a straightforward chemical doping scenario and occurs in conjunction with profound changes in the initial states and/or spatial distribution of near-E(F) electrons in the surface region.

Role of lattice coupling in establishing electronic and magnetic properties in quasi-one-dimensional cuprates.

High resolution resonant inelastic x-ray scattering has been performed to reveal the role of lattice coupling in a family of quasi-1D insulating cuprates, Ca2+5xY2-5xCu5O10. Site-dependent low-energy excitations arising from progressive emissions of a 70 meV lattice vibrational mode are resolved for the first time, providing a direct measurement of electron-lattice coupling strength. We show that such electron-lattice coupling causes doping-dependent distortions of the Cu-O-Cu bond angle, which sets the intrachain spin exchange interactions. Our results indicate that the lattice degrees of freedom are fully integrated into the electronic behavior in low-dimensional systems.

Real-time manifestation of strongly coupled spin and charge order parameters in stripe-ordered La(1.75)Sr(0.25)NiO(4) nickelate crystals using time-resolved resonant x-ray diffraction.

We investigate the order parameter dynamics of the stripe-ordered nickelate, La(1.75)Sr(0.25)NiO(4), using time-resolved resonant x-ray diffraction. In spite of distinct spin and charge energy scales, the two order parameters' amplitude dynamics are found to be linked together due to strong coupling. Additionally, the vector nature of the spin sector introduces a longer reorientation time scale which is absent in the charge sector. These findings demonstrate that the correlation linking the symmetry-broken states does not unbind during the nonequilibrium process, and the time scales are not necessarily associated with the characteristic energy scales of individual degrees of freedom.

Three-dimensional spin rotations at the Fermi surface of a strongly spin-orbit coupled surface system.

The spin texture of the metallic two-dimensional electron system (sqrt[3]×sqrt[3])-Au/Ge(111) is revealed by fully three-dimensional spin-resolved photoemission, as well as by density functional calculations. The large hexagonal Fermi surface, generated by the Au atoms, shows a significant splitting due to spin-orbit interactions. The planar components of the spin exhibit a helical character, accompanied by a strong out-of-plane spin component with alternating signs along the six Fermi surface sections. Moreover, in-plane spin rotations toward a radial direction are observed close to the hexagon corners. Such a threefold-symmetric spin pattern is not described by the conventional Rashba model. Instead, it reveals an interplay with Dresselhaus-like spin-orbit effects as a result of the crystalline anisotropies.

Bulk electronic structure of superconducting LaRu2P2 single crystals measured by soft-X-ray angle-resolved photoemission spectroscopy.

We present a soft x-ray angle-resolved photoemission spectroscopy (SX-ARPES) study of the stoichiometric pnictide superconductor LaRu(2)P(2). The observed electronic structure is in good agreement with density functional theory (DFT) calculations. However, it is significantly different from its counterpart in high-temperature superconducting Fe pnictides. In particular, the bandwidth renormalization present in the Fe pnictides (~2-3) is negligible in LaRu(2)P(2) even though the mass enhancement is similar in both systems. Our results suggest that the superconductivity in LaRu(2) P(2) has a different origin with respect to the iron pnictides. Finally, we demonstrate that the increased probing depth of SX-ARPES, compared to the widely used ultraviolet ARPES, is essential in determining the bulk electronic structure in the experiment.

Nature of weak magnetism in SrTiO3/LaAlO3 multilayers.

We report the observation of weak magnetism in superlattices of LaAlO(3)/SrTiO(3) using ß-detected nuclear magnetic resonance. The spin lattice relaxation rate of ^{8}Li in superlattices with a spacer layers of 8 and 6 unit cells of LaAlO(3) exhibits a strong peak near ~35 K, whereas no such peak is observed in a superlattice with spacer layer thickness of 3 unit cells. We attribute the observed temperature dependence to slowing down of weakly coupled electronic moments at the LaAlO(3)/SrTiO(3) interface. These results show that the magnetism at the interface depends strongly on the thickness of the spacer layer, and that a minimal thickness of ~4-6 unit cells is required for the appearance of magnetism. A simple model is used to determine that the observed relaxation is due to small fluctuating moments (~0.002µ(B)) in the two samples with a larger LaAlO(3) spacer thickness.

Femtosecond dynamics of the collinear-to-spiral antiferromagnetic phase transition in CuO.

We report on the ultrafast dynamics of magnetic order in a single crystal of CuO at a temperature of 207 K in response to strong optical excitation using femtosecond resonant x-ray diffraction. In the experiment, a femtosecond laser pulse induces a sudden, nonequilibrium increase in magnetic disorder. After a short delay ranging from 400 fs to 2 ps, we observe changes in the relative intensity of the magnetic ordering diffraction peaks that indicate a shift from a collinear commensurate phase to a spiral incommensurate phase. These results indicate that the ultimate speed for this antiferromagnetic reorientation transition in CuO is limited by the long-wavelength magnetic excitation connecting the two phases.

Numerical optimization of spherical variable-line-spacing grating X-ray spectrometers.

Operation of an X-ray spectrometer based on a spherical variable-line-spacing (VLS) grating is analyzed using dedicated ray-tracing software allowing fast optimization of the grating parameters and spectrometer geometry. The analysis is illustrated with optical design of a model spectrometer to deliver a resolving power above 20400 at a photon energy of 930 eV (Cu L-edge). With this energy taken as reference, the VLS coefficients are optimized to cancel the lineshape asymmetry (mostly from the coma aberrations) as well as minimize the symmetric aberration broadening at large grating illuminations, dramatically increasing the aberration-limited vertical acceptance of the spectrometer. For any energy away from the reference, corrections to the entrance arm and light incidence angle on the grating are evaluated to maintain the exactly symmetric lineshape. Furthermore, operational modes when these corrections are coordinated are evaluated to maintain either energy-independent focal curve inclination or maximal aberration-limited spectrometer acceptance. The results are supported by analytical evaluation of the coma term of the optical path function. This analysis thus gives a recipe for designing a high-resolution spherical VLS grating spectrometer operating with negligible aberrations at large acceptance and over an extended energy range.

Insight into the f-derived Fermi surface of the heavy-fermion compound YbRh2Si2.

Angle-resolved photoelectron spectroscopy (ARPES) was used to study the Fermi surface of the heavy-fermion system YbRh(2)Si(2) at a temperature of about 10 K, i.e., a factor of 2 below the Kondo energy scale. We observed sharp structures with a well-defined topology, which were analyzed by comparing with results of band-structure calculations based on the local-density approximation (LDA). The observed bulk Fermi surface presents strong similarities with that expected for a trivalent Yb state, but is slightly larger, has a strong Yb-4f character, and deviates from the LDA results by a larger region without states around the Γ point. These properties are qualitatively explained in the framework of a simple f-d hybridization model. Our analysis highlights the importance of taking into account surface states and doing an appropriate projection along k(z) when comparing ARPES data with results from theoretical calculations.

Strain wave pathway to semiconductor-to-metal transition revealed by time-resolved X-ray powder diffraction.

One of the main challenges in ultrafast material science is to trigger phase transitions with short pulses of light. Here we show how strain waves, launched by electronic and structural precursor phenomena, determine a coherent macroscopic transformation pathway for the semiconducting-to-metal transition in bistable Ti3O5 nanocrystals. Employing femtosecond powder X-ray diffraction, we measure the lattice deformation in the phase transition as a function of time. We monitor the early intra-cell distortion around the light absorbing metal dimer and the long range deformations governed by acoustic waves propagating from the laser-exposed Ti3O5 surface. We developed a simplified elastic model demonstrating that picosecond switching in nanocrystals happens concomitantly with the propagating acoustic wavefront, several decades faster than thermal processes governed by heat diffusion.

High-resolution soft X-ray beamline ADRESS at the Swiss Light Source for resonant inelastic X-ray scattering and angle-resolved photoelectron spectroscopies.

The concepts and technical realisation of the high-resolution soft X-ray beamline ADRESS operating in the energy range from 300 to 1600 eV and intended for resonant inelastic X-ray scattering (RIXS) and angle-resolved photoelectron spectroscopy (ARPES) are described. The photon source is an undulator of novel fixed-gap design where longitudinal movement of permanent magnetic arrays controls not only the light polarization (including circular and 0-180 degrees rotatable linear polarizations) but also the energy without changing the gap. The beamline optics is based on the well established scheme of plane-grating monochromator operating in collimated light. The ultimate resolving power E/DeltaE is above 33000 at 1 keV photon energy. The choice of blazed versus lamellar gratings and optimization of their profile parameters is described. Owing to glancing angles on the mirrors as well as optimized groove densities and profiles of the gratings, the beamline is capable of delivering high photon flux up to 1 x 10(13) photons s(-1) (0.01% BW)(-1) at 1 keV. Ellipsoidal refocusing optics used for the RIXS endstation demagnifies the vertical spot size down to 4 microm, which allows slitless operation and thus maximal transmission of the high-resolution RIXS spectrometer delivering E/DeltaE > 11000 at 1 keV photon energy. Apart from the beamline optics, an overview of the control system is given, the diagnostics and software tools are described, and strategies used for the optical alignment are discussed. An introduction to the concepts and instrumental realisation of the ARPES and RIXS endstations is given.

k Dependence of the crystal-field splittings of 4f states in rare-earth systems.

The occupation, energy separation, and order of the crystal-field-split 4f states are crucial for the understanding of the magnetic properties of rare-earth systems. We provide the experimental evidence that crystal-field-split 4f states exhibit energy dispersion in momentum space leading to variations of energy spacings between them and even of their energy sequence across the Brillouin zone. These observations were made by performing angle-resolved photoemission experiments on YbRh(2)Si(2) and properly simulated within a simple model based on results obtained by inelastic neutron scattering experiments and band structure calculations. Our findings should be generally applicable to rare-earth systems and have considerable impact on the understanding of magnetism and related phenomena.

Observation of time-reversal-protected single-dirac-cone topological-insulator states in Bi2Te3 and Sb2Te3.

We show that the strongly spin-orbit coupled materials Bi2Te3 and Sb2Te3 and their derivatives belong to the Z2 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 (delta approximately 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 spin-Dirac fermions can be controlled through systematic Mn doping, making these materials classes potentially suitable for topological device applications.