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Homogeneous mixed-valence (MV) behaviour is one of the most intriguing phenomena of f-electron systems. Despite extensive efforts, a fundamental aspect which remains unsettled is the experimental determination of the limiting cases for which MV emerges. Here we address this question for SmB6, a prototypical MV system characterized by two nearly-degenerate Sm2+ and Sm3+ configurations. By combining angle-resolved photoemission spectroscopy (ARPES) and x-ray absorption spectroscopy (XAS), we track the evolution of the mean Sm valence, vSm, in the SmxLa1-xB6 series. Upon substitution of Sm ions with trivalent La, we observe a linear decrease of valence fluctuations to an almost complete suppression at x = 0.2, with vSm ~ 2; surprisingly, by further reducing x, a re-entrant increase of vSm develops, approaching the value of vimp ~ 2.35 in the dilute-impurity limit. Such behaviour departs from a monotonic evolution of vSm across the whole series, as well as from the expectation of its convergence to an integer value for x â 0. Our ARPES and XAS results, complemented by a phenomenological model, demonstrate an unconventional evolution of the MV character in the SmxLa1-xB6 series, paving the way to further theoretical and experimental considerations on the concept of MV itself, and its influence on the macroscopic properties of rare-earth compounds in the dilute-to-intermediate impurity regime.
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In spintronics, the two main approaches to actively control the electrons' spin involve static magnetic or electric fields. An alternative avenue relies on the use of optical fields to generate spin currents, which can bolster spin-device performance, allowing for faster and more efficient logic. To date, research has mainly focused on the optical injection of spin currents through the photogalvanic effect, and little is known about the direct optical control of the intrinsic spin-splitting. To explore the optical manipulation of a material's spin properties, we consider the Rashba effect. Using time- and angle-resolved photoemission spectroscopy (TR-ARPES), we demonstrate that an optical excitation can tune the Rashba-induced spin splitting of a two-dimensional electron gas at the surface of Bi2Se3. We establish that light-induced photovoltage and charge carrier redistribution - which in concert modulate the Rashba spin-orbit coupling strength on a sub-picosecond timescale - can offer an unprecedented platform for achieving optically-driven spin logic devices.
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Time-resolved photoemission with ultrafast pump and probe pulses is an emerging technique with wide application potential. Real-time recording of nonequilibrium electronic processes, transient states in chemical reactions, or the interplay of electronic and structural dynamics offers fascinating opportunities for future research. Combining valence-band and core-level spectroscopy with photoelectron diffraction for electronic, chemical, and structural analyses requires few 10 fs soft X-ray pulses with some 10 meV spectral resolution, which are currently available at high repetition rate free-electron lasers. We have constructed and optimized a versatile setup commissioned at FLASH/PG2 that combines free-electron laser capabilities together with a multidimensional recording scheme for photoemission studies. We use a full-field imaging momentum microscope with time-of-flight energy recording as the detector for mapping of 3D band structures in (kx, ky, E) parameter space with unprecedented efficiency. Our instrument can image full surface Brillouin zones with up to 7 Å-1 diameter in a binding-energy range of several eV, resolving about 2.5 × 105 data voxels simultaneously. Using the ultrafast excited state dynamics in the van der Waals semiconductor WSe2 measured at photon energies of 36.5 eV and 109.5 eV, we demonstrate an experimental energy resolution of 130 meV, a momentum resolution of 0.06 Å-1, and a system response function of 150 fs.
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Magnetotransport constitutes a useful probe to understand the interplay between electronic band topology and magnetism in spintronic devices. A recent theory of Lu and Shen [Phys. Rev. Lett. 112, 146601 (2014)PRLTAO0031-900710.1103/PhysRevLett.112.146601] on magnetically doped topological insulators predicts that quantum corrections Δκ to the temperature dependence of conductivity can change sign across the Curie transition. This phenomenon has been attributed to a suppression of the Berry phase of the topological surface states at the Fermi level, caused by a magnetic energy gap. Here, we demonstrate experimentally that Δκ can reverse its sign even when the Berry phase at the Fermi level remains unchanged. The contradictory behavior to theory predictions is resolved by extending the model by Lu and Shen to a nonmonotonic temperature scaling of the inelastic scattering length showing a turning point at the Curie transition.
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PURPOSE: Cerebellar herniation in Chiari patients can be dynamic, following the cerebrospinal fluid pulsatility during the cardiac cycle. We present a voxel intensity distribution method (VIDM) to automatically extract the pulsatility-dependent herniation in time-resolved MRI (CINE MRI) and compare it to the simple linear measurements. The degree of herniation is furthermore compared on CINE and static sequences, and the cerebellar movement is correlated to the presence of hydrocephalus and syringomyelia. METHODS: The cerebellar movement in 27 Chiari patients is analyzed with VIDM and the results were compared to linear measurements on an image viewer (visual inspection, VI) using a paired t test. Second, an ANOVA test is applied to compare the degree of herniation on static 3D MRI and CINE. Finally, the Pearson's correlation coefficient is calculated for the correlation between cerebellar movement and the presence of hydrocephalus and syringomyelia. RESULTS: VIDM showed significant movement in 85% of our patients. Assuming that movement < 1 mm cannot be detected reliably on an image viewer, VI identified movement in 29.6% of the patients (p = 0.002). The herniation was greater on static sequences than on CINE in most cases, but this was not statistically significant. The cerebellar movement was not correlated with hydrocephalus or syringomyelia (Pearson's coefficient < 0.3). CONCLUSIONS: VIDM is a sensitive method to detect tissue movement on CINE MRI and could be used for Chiari patients, but also for the evaluation of cyst membranes, ventriculostomies, etc. The cerebellar movement appears not to correlate with hydrocephalus and syringomyelia in Chiari patients.
Assuntos
Malformação de Arnold-Chiari/diagnóstico por imagem , Cerebelo/diagnóstico por imagem , Imagem Cinética por Ressonância Magnética , Malformação de Arnold-Chiari/patologia , Cerebelo/patologia , Criança , Feminino , Humanos , Imageamento Tridimensional , Masculino , Estudos RetrospectivosRESUMO
We demonstrate simultaneous quantization of conduction band (CB) and valence band (VB) states in silicon using ultrashallow, high-density, phosphorus doping profiles (so-called Si:P δ layers). We show that, in addition to the well-known quantization of CB states within the dopant plane, the confinement of VB-derived states between the subsurface P dopant layer and the Si surface gives rise to a simultaneous quantization of VB states in this narrow region. We also show that the VB quantization can be explained using a simple particle-in-a-box model, and that the number and energy separation of the quantized VB states depend on the depth of the P dopant layer beneath the Si surface. Since the quantized CB states do not show a strong dependence on the dopant depth (but rather on the dopant density), it is straightforward to exhibit control over the properties of the quantized CB and VB states independently of each other by choosing the dopant density and depth accordingly, thus offering new possibilities for engineering quantum matter.
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The discovery of high-temperature superconductivity in Fe-based compounds triggered numerous investigations on the interplay between superconductivity and magnetism, and on the enhancement of transition temperatures through interface effects. It is widely believed that the emergence of optimal superconductivity is intimately linked to the suppression of long-range antiferromagnetic (AFM) order, although the exact microscopic picture remains elusive because of the lack of atomically resolved data. Here we present spin-polarized scanning tunnelling spectroscopy of ultrathin FeTe1-xSex (x=0, 0.5) films on bulk topological insulators. Surprisingly, we find an energy gap at the Fermi level, indicating superconducting correlations up to Tcâ¼6 K for one unit cell FeTe grown on Bi2Te3, in contrast to the non-superconducting bulk FeTe. The gap spatially coexists with bi-collinear AFM order. This finding opens perspectives for theoretical studies of competing orders in Fe-based superconductors and for experimental investigations of exotic phases in superconducting layers on topological insulators.
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A combined experimental and theoretical study of doping individual Fe atoms into Bi(2)Se(3) is presented. It is shown through a scanning tunneling microscopy study that single Fe atoms initially located at hollow sites on top of the surface (adatoms) can be incorporated into subsurface layers by thermally activated diffusion. Angle-resolved photoemission spectroscopy in combination with ab initio calculations suggest that the doping behavior changes from electron donation for the Fe adatom to neutral or electron acceptance for Fe incorporated into substitutional Bi sites. According to first principles calculations within density functional theory, these Fe substitutional impurities retain a large magnetic moment, thus presenting an alternative scheme for magnetically doping the topological surface state. For both types of Fe doping, we see no indication of a gap at the Dirac point.
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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.
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The robustness of the gapless topological surface state hosted by a 3D topological insulator against perturbations of magnetic origin has been the focus of recent investigations. We present a comprehensive study of the magnetic properties of Fe impurities on the prototypical 3D topological insulator Bi(2)Se(3) using local low-temperature scanning tunneling spectroscopy and integral x-ray magnetic circular dichroism techniques. Single Fe adatoms on the Bi(2)Se(3) surface, in the coverage range ≈ 1% of a monolayer, are heavily relaxed into the surface and exhibit a magnetic easy axis within the surface plane, contrary to what was assumed in recent investigations on the supposed opening of a gap. Using ab initio approaches, we demonstrate that an in-plane easy axis arises from the combination of the crystal field and dynamic hybridization effects.
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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.
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An energy gap between the valence and the conduction band is the defining property of a semiconductor, and the gap size plays a crucial role in the design of semiconductor devices. We show that the presence of a two-dimensional electron gas near to the surface of a semiconductor can significantly alter the size of its band gap through many-body effects caused by its high electron density, resulting in a surface band gap that is much smaller than that in the bulk. Apart from reconciling a number of disparate previous experimental findings, the results suggest an entirely new route to spatially inhomogeneous band-gap engineering.
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The self-assembly of organic molecules on surfaces is a promising approach for the development of nanoelectronic devices. Although a variety of strategies have been used to establish stable links between molecules, little is known about the electrical conductance of these links. Extended electronic states, a prerequisite for good conductance, have been observed for molecules adsorbed on metal surfaces. However, direct conductance measurements through a single layer of molecules are only possible if the molecules are adsorbed on a poorly conducting substrate. Here we use a nanoscale four-point probe to measure the conductivity of a self-assembled layer of cobalt phthalocyanine on a silver-terminated silicon surface as a function of thickness. For low thicknesses, the cobalt phthalocyanine molecules lie flat on the substrate, and their main effect is to reduce the conductivity of the substrate. At higher thicknesses, the cobalt phthalocyanine molecules stand up to form stacks and begin to conduct. These results connect the electronic structure and orientation of molecular monolayer and few-layer systems to their transport properties, and should aid in the rational design of future devices.
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The (114) surface of the semimetal Bi is found to support a quasi-one-dimensional, metallic surface state. As required by symmetry, the state is degenerate along the Gamma-Y line of the surface Brillouin zone with a highest binding energy of approximately 150 meV. In the Gamma-X direction the degeneracy is lifted by the strong spin-orbit splitting in Bi, as directly shown by spin-resolved photoemission. This results in a Fermi contour consisting of two closely separated, parallel lines of opposite spin direction. It is argued that similar states on related insulators would give rise to a one-dimensional quantum spin Hall effect.
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Several approaches for surface-sensitive conductance measurements are reviewed. Particular emphasis is placed on nanoscale multi-point probe techniques. The results for two model systems, which have given rise to some dispute, are discussed in detail: Si(111)(7 × 7) and ([Formula: see text])Ag-Si(111). Other recent examples are also given, such as phase transitions in quasi-one-dimensional structures on semiconductor surfaces and the surface sheet conductivity of Bi(111), the surface of a semimetal.
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The temperature-dependent surface conductivity of the Si(111)([Formula: see text])Ag surface was measured using a microscopic four-point probe. The conductivity was found to undergo a sharp increase of about three orders of magnitude when the system was heated above about 220 K. This strong conductivity change is reversible and attributed to the phase transition which is generally believed to occur on this surface. It is also shown that, in order to find the true surface conductivity, it is necessary to separate it from the contribution of the bulk and space charge layer. In this work, this is achieved by using a finite-element model. A percolating network of Ag islands on Si(111) was also studied and a much simpler behaviour (compared to that of Si(111)([Formula: see text])Ag) was found. The temperature-dependent conductivity of this system was found to display typical metallic behaviour. The absolute value of the conductivity is comparable to the value expected by modelling the Ag film as exhibiting the bulk Ag transport properties.
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A novel approach for extracting genuine surface conductivities is presented and illustrated using the unresolved example of Si(111)-(7 x 7). Its temperature-dependent conductivity was measured with a microscopic four point probe between room temperature and 100 K. At room temperature the measured conductance corresponds to that expected from the bulk doping level. However, as the temperatures is lowered below approximately 200 K, the conductance decreases by several orders of magnitude in a small temperature range and it saturates at a low temperature value of approximately 4 x 10(-8) Omega(-1), irrespective of bulk doping. This abrupt transition is interpreted as the switching from bulk to surface conduction, an interpretation which is supported by a numerical model for the measured four point probe conductance. The value of the surface conductance is considerably lower than that of a good metal.
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Quasiparticle interference patterns measured by scanning tunneling microscopy can be used to study the local electronic structure of metal surfaces and high-temperature superconductors. Here, we show that even in nonmagnetic systems the spin of the quasiparticles can have a profound effect on the interference patterns. On Bi(110), where the surface state bands are not spin degenerate, the patterns are not related to the dispersion of the electronic states in a simple way. In fact, the features which are expected for the spin-independent situation are absent and the observed interference patterns can be interpreted only by taking spin-conserving scattering events into account.