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The extension of transient grating spectroscopy to the x-ray regime will create numerous opportunities, ranging from the study of thermal transport in the ballistic regime to charge, spin, and energy transfer processes with atomic spatial and femtosecond temporal resolution. Studies involving complicated split-and-delay lines have not yet been successful in achieving this goal. Here we propose a novel, simple method based on the Talbot effect for converging beams, which can easily be implemented at current x-ray free electron lasers. We validate our proposal by analyzing printed interference patterns on polymethyl methacrylate and gold samples using â¼3 keV X-ray pulses.
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Blazed gratings are of dedicated interest for the monochromatization of synchrotron radiation when a high photon flux is required, such as, for example, in resonant inelastic X-ray scattering experiments or when the use of laminar gratings is excluded due to too high flux densities and expected damage, for example at free-electron laser beamlines. Their availability became a bottleneck since the decommissioning of the grating manufacture facility at Carl Zeiss in Oberkochen. To resolve this situation a new technological laboratory was established at the Helmholtz Zentrum Berlin, including instrumentation from Carl Zeiss. Besides the upgraded ZEISS equipment, an advanced grating production line has been developed, including a new ultra-precise ruling machine, ion etching technology as well as laser interference lithography. While the old ZEISS ruling machine GTM-6 allows ruling for a grating length up to 170â mm, the new GTM-24 will have the capacity for 600â mm (24â inch) gratings with groove densities between 50â linesâ mm-1 and 1200â linesâ mm-1. A new ion etching machine with a scanning radiofrequency excited ion beam (HF) source allows gratings to be etched into substrates of up to 500â mm length. For a final at-wavelength characterization, a new reflectometer at a new Optics beamline at the BESSY-II storage ring is under operation. This paper reports on the status of the grating fabrication, the measured quality of fabricated items by ex situ and in situ metrology, and future development goals.
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The distribution of valence electrons in metals usually follows the symmetry of the underlying ionic lattice. Modulations of this distribution often occur when those electrons are not stable with respect to a new electronic order, such as spin or charge density waves. Electron density waves have been observed in many families of superconductors, and are often considered to be essential for superconductivity to exist. Recent measurements seem to show that the properties of the iron pnictides are in good agreement with band structure calculations that do not include additional ordering, implying no relation between density waves and superconductivity in these materials. Here we report that the electronic structure of Ba(1-x)K(x)Fe(2)As(2) is in sharp disagreement with those band structure calculations, and instead reveals a reconstruction characterized by a (pi, pi) wavevector. This electronic order coexists with superconductivity and persists up to room temperature (300 K).
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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.
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The single-layered half-doped manganite La(0.5)Sr(1.5)MnO4 (LSMO), was studied by means of the angle-resolved photoemission spectroscopy (ARPES), scanning tunneling microscopy (STM), and resistivity measurements. STM revealed a smooth reconstruction-free surface; the density of states, extracted from photoemission and tunneling spectroscopy, is in agreement with transport measurements. The derived from ARPES Fermi surface (FS) nesting properties correspond to the known pattern of the charge-orbital ordering (COO), which implies that FS instability is related to the propensity to form a COO state in LSMO.
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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.
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We have studied the electronic structure of the nonmagnetic LiFeAs (T(c)â¼18 K) superconductor using angle-resolved photoemission spectroscopy. We find a notable absence of the Fermi surface nesting, strong renormalization of the conduction bands by a factor of 3, high density of states at the Fermi level caused by a van Hove singularity, and no evidence for either a static or a fluctuating order except superconductivity with in-plane isotropic energy gaps. Our observations suggest that these electronic properties capture the majority of ingredients necessary for the superconductivity in iron pnictides.
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As a homologue to the new, Fe-based type of high-temperature superconductors, the electronic structure of the heavy-fermion compound CeFePO was studied by means of angle-resolved resonant photoemission. It was experimentally found-and later on confirmed by local-density approximation (LDA) as well as dynamical mean-field theory (DMFT) calculations-that the Ce 4f states hybridize to the Fe 3d states of d{3z{2}-r{2}} symmetry near the Fermi level that discloses their participation in the occurring electron-correlation phenomena and provides insight into mechanism of superconductivity in oxopnictides.
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Photoionization (PI) of Fe14+ in the range from 450 to 1100 eV was measured at the BESSY II storage ring using an electron beam ion trap achieving high target-ion area densities of 10(10) cm(-2). Photoabsorption by this ion is observed in astrophysical spectra and plasmas, but until now cross sections and resonance energies could only be provided by calculations. We reach a resolving power E/ΔE of at least 6500, outstanding in the present energy range, which enables benchmarking and improving the most advanced theories for PI of ions in high charge states.
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Electron-hybridization phenomena in YbRh_{2}Si_{2} were probed by angle-resolved photoemission. It was shown that the Yb 4f-Rh 4d hybridization strength in the surface region of this heavy-fermion material can be varied by deposition of Ag. Site-specific charge transfer from adatoms leads to change of the energy overlap of the interacting states close to the Fermi energy. Our study demonstrates a new way to tune the hybridization between 4f and valence electrons as well as the induced strong correlation effects at the surface of heavy-fermion systems.
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Using angle-resolved photoemission spectroscopy, we report on the direct observation of the energy gap in 2H-NbSe2 caused by the charge-density waves (CDW). The gap opens in the regions of the momentum space connected by the CDW vectors, which implies a nesting mechanism of CDW formation. In remarkable analogy with the pseudogap in cuprates, the detected energy gap also exists in the normal state (T>T0) where it breaks the Fermi surface into "arcs," it is nonmonotonic as a function of temperature with a local minimum at the CDW transition temperature (T0), and it forestalls the superconducting gap by excluding the nested portions of the Fermi surface from participating in superconductivity.
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We present a variable line-space grating spectrometer for soft x-rays that covers the photon energy range between 130 and 650 eV. The optical design is based on the Hettrick-Underwood principle and tailored to synchrotron-based studies of radiation-sensitive biological samples. The spectrometer is able to record the entire spectral range in one shot, i.e., without any mechanical motion, at a resolving power of 1200 or better. Despite its slitless design, such a resolving power can be achieved for a source spot as large as (30 x 3000) microm2, which is important for keeping beam damage effects in radiation-sensitive samples low. The high spectrometer efficiency allows recording of comprehensive two-dimensional resonant inelastic soft x-ray scattering (RIXS) maps with good statistics within several minutes. This is exemplarily demonstrated for a RIXS map of highly oriented pyrolytic graphite, which was taken within 10 min.
Assuntos
Espectrometria por Raios X/instrumentação , Algoritmos , Desenho de Equipamento , Fótons , Espalhamento de Radiação , Raios XRESUMO
The mixed-valent compound EuNi2P2 was studied by photoemission. Observed splittings and dispersions of the Eu 4f;{6} final state close to energy crossings of the Eu 4f and Ni 3d states are explained in terms of hybridization by a momentum and energy dependence of the electron hopping matrix element. These data obtained for a system with more than one 4f electron (hole) show that dispersions and hybridization gaps related to Kondo and heavy-fermion behavior can be found in other rare-earth-metal compounds apart from Ce and Yb-based ones.
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Measurements of the low-energy electronic structure in Gd2PdSi3 and Tb2PdSi3 by means of angle-resolved photoelectron spectroscopy reveal a Fermi surface consisting of an electron barrel at the Gamma point surrounded by spindle-shaped electron pockets originating from the same band. The calculated momentum-dependent RKKY coupling strength is peaked at the 1/2GammaK wave vector, which coincides with the propagation vector of the low-temperature in-plane magnetic order observed by neutron diffraction, thereby demonstrating the decisive role of the Fermi surface geometry in explaining the complex magnetic ground state of ternary rare earth silicides.
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We present a calculation of the Hall coefficient in 2H-TaSe(2) and 2H-Cu(0.2)NbS(2) based on their electronic structure extracted from angle-resolved photoemission spectra. The well-known semiclassical approach, based on the solution of the Boltzmann equation, yields the correct value for the normal-state Hall coefficient. Entering the charge density wave state results in the opening of the pseudogap and redistribution of the spectral weight. Accounting for this allows us to reproduce the temperature dependence of the Hall coefficient, including the prominent sign change, with no adjustable parameters.
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The full three-dimensional dispersion of the pi bands, Fermi velocities, and effective masses are measured with angle-resolved photoemission spectroscopy and compared to first-principles calculations. The band structure by density-functional theory underestimates the slope of the bands and the trigonal warping effect. Including electron-electron correlation on the level of the GW approximation, however, yields remarkable improvement in the vicinity of the Fermi level. This demonstrates the breakdown of the independent electron picture in semimetallic graphite and points toward a pronounced role of electron correlation for the interpretation of transport experiments and double-resonant Raman scattering for a wide range of carbon based materials.
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Using angle-resolved photoemission spectroscopy we demonstrate that a normal-state pseudogap exists above T(N-IC) in one of the most studied two-dimensional charge-density wave (CDW) dichalcogenides 2H-TaSe(2). The initial formation of the incommensurate CDW is confirmed as being driven by a conventional nesting instability, which is marked by a pseudogap. The magnitude, character, and anisotropy of the 2D-CDW pseudogap bear considerable resemblance to those seen in superconducting cuprates.
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Using high-resolution angle-resolved photoemission spectroscopy we have studied the momentum and photon energy dependence of the anomalous high-energy dispersion, termed waterfalls, between the Fermi level and 1 eV binding energy in several high-T_{c} superconductors. We observe strong changes of the dispersion between different Brillouin zones and a strong dependence on the photon energy around 75 eV, which we associate with the resonant photoemission at the Cu3p-->3d_{x;{2}-y;{2}} edge. We conclude that the high-energy "waterfall" dispersion results from a strong suppression of the photoemission intensity at the center of the Brillouin zone due to matrix element effects and is, therefore, not an intrinsic feature of the spectral function. This indicates that the new high-energy scale in the electronic structure of cuprates derived from the waterfall-like dispersion may be incorrect.
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We apply the new-generation angle-resolved photoemission spectroscopy methodology to the most widely studied cuprate superconductor YBa2Cu3O(6+x). Considering the nodal direction, we found noticeable renormalization effects known as kinks both in the quasiparticle dispersion and scattering rate, the bilayer splitting, and evidence for strong interband scattering--all the characteristic features of the nodal quasiparticles detected earlier in Bi2Sr2CaCu2O(8+delta). The typical energy scale and the doping dependence of the kinks clearly point to their intimate relation with the spin-1 resonance seen in the neutron scattering experiments. Our findings strongly suggest a universality of the electron dynamics in the bilayer superconducting cuprates and a dominating role of the spin fluctuations in the formation of the quasiparticles along the nodal direction.
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The Cu substitution by Zn and Ni impurities and its influence on the mass renormalization effects in angle-resolved photoelectron spectra (ARPES) of Bi2Sr2CaCu2O8-delta is addressed. We show that the nonmagnetic Zn atoms have a much stronger effect in both the nodal and antinodal parts of the Brillouin zone than magnetic Ni. The observed changes are consistent with the behavior of the spin resonance mode as seen by inelastic neutron scattering in YBCO. This strongly suggests that the "peak-dip-hump" and the kink in ARPES on the one side and neutron resonance on the other are closely related features.