Hole-depletion of ladders in Sr14_{14}Cu24_{24}O41_{41} induced by correlation effects

The hole distribution in Sr$_{14}$Cu$_{24}$O$_{41}$ is studied by low temperature polarization dependent O K Near-Edge X-ray Absorption Fine Structure measurements and state of the art electronic structure calculations that include core-hole and correlation effects in a mean-field approach. Contrary to all previous analysis, based on semi-empirical models, we show that correlations and antiferromagnetic ordering favor the strong chain hole-attraction. For the remaining small number of holes accommodated on ladders, leg-sites are preferred to rung-sites. The small hole affinity of rung-sites explains naturally the 1D - 2D cross-over in the phase diagram of (La,Y,Sr,Ca)$_{14}$Cu$_{24}$O$_{41}$Comment: 6 pages, 8 figure

Fermi Surface and Quasiparticle Excitations of overdoped Tl2Ba2CuO6+d by ARPES

The electronic structure of the high-T_c superconductor Tl2Ba2CuO6+d is studied by ARPES. For a very overdoped Tc=30K sample, the Fermi surface consists of a single large hole pocket centered at (pi,pi) and is approaching a topological transition. Although a superconducting gap with d_x^2-y^2 symmetry is tentatively identified, the quasiparticle evolution with momentum and binding energy exhibits a marked departure from the behavior observed in under and optimally doped cuprates. The relevance of these findings to scattering, many-body, and quantum-critical phenomena is discussed.Comment: Revised manuscript, in press on PRL. A high-resolution version can be found at http://www.physics.ubc.ca/~quantmat/ARPES/PUBLICATIONS/Articles/Tl2201_LE.pdf and related material at http://www.physics.ubc.ca/~quantmat/ARPES/PUBLICATIONS/articles.htm

Emergent c-axis magnetic helix in manganite-nickelate superlattices

The nature of the magnetic order in (La2/3Sr1/3MnO3)9/(LaNiO3)3 superlattices is investigated using x-ray resonant magnetic reflectometry. We observe a new c-axis magnetic helix state in the (LaNiO3)3 layers that had never been reported in nickelates, and which mediates the ~130deg magnetic coupling between the ferromagnetic (La2/3Sr1/3MnO3)9 layers, illustrating the power of x-rays for discovering the magnetic state of complex oxide interfaces. Resonant inelastic x-ray scattering and x-ray absorption spectroscopy show that Ni-O ligand hole states from bulk LaNiO3 are mostly filled due to interfacial electron transfer from Mn, driving the Ni orbitals closer to an atomic-like 3d8 configuration. We discuss the constraints imposed by this electronic configuration to the microscopic origin of the observed magnetic structure. The presence of a magnetic helix in (La2/3Sr1/3MnO3)9/(LaNiO3)3 is crucial for modeling the potential spintronic functionality of this system and may be important for designing emergent magnetism in novel devices in general.Comment: 7 pages, 5 figure

Resonant inelastic x-ray scattering data for Ruddlesden-Popper and reduced Ruddlesden-Popper nickelates

Ruddlesden-Popper and reduced Ruddlesden-Popper nickelates are intriguing candidates for mimicking the properties of high-temperature superconducting cuprates. The degree of similarity between these nickelates and cuprates has been the subject of considerable debate. Resonant inelastic x-ray scattering (RIXS) has played an important role in exploring their electronic and magnetic excitations, but these efforts have been stymied by inconsistencies between different samples and the lack of publicly available data for detailed comparison. To address this issue, we present open RIXS data on La4Ni3O10 and La4Ni3O8.Comment: Data descriptor article; accepted in Scientific Data; 8 pages; 6 figure

Electronic structure of a Mn12 molecular magnet: Theory and experiment

金沢大学大学院自然科学研究科物質情報解析We used site-selective and element-specific resonant inelastic x-ray scattering (RIXS) to study the electronic structure and the electron interaction effects in the molecular magnet [Mn12 O12 (C H3 COO)16 (H2 O)4] 2C H3 COOH 4 H2 O, and compared the experimental data with the results of local spin density approximation +U electron structure calculations which include the on-site Coulomb interactions. We found a good agreement between theory and experiment for the Coulomb repulsion parameter U=4 eV. In particular, the p-d band separation of 1.8 eV has been found from the RIXS spectra, which is in accordance with the calculations. Similarly, the positions of the peaks in the XPS spectra agree with the calculated densities of p and d states. Using the results of the electronic structure calculations, we determined the intramolecular exchange parameters, and used them for diagonalization of the Mn12 spin Hamiltonian. The calculated exchanges gave the correct ground state with the total spin S=10. © 2007 The American Physical Society

Electron population dynamics in resonant non-linear x-ray absorption in nickel at a free-electron laser

Free-electron lasers provide bright, ultrashort, and monochromatic x-ray pulses, enabling novel spectroscopic measurements not only with femtosecond temporal resolution: The high fluence of their x-ray pulses can also easily enter the regime of the non-linear x-ray–matter interaction. Entering this regime necessitates a rigorous analysis and reliable prediction of the relevant non-linear processes for future experiment designs. Here, we show non-linear changes in the L3-edge absorption of metallic nickel thin films, measured with fluences up to 60 J/cm2. We present a simple but predictive rate model that quantitatively describes spectral changes based on the evolution of electronic populations within the pulse duration. Despite its simplicity, the model reaches good agreement with experimental results over more than three orders of magnitude in fluence, while providing a straightforward understanding of the interplay of physical processes driving the non-linear changes. Our findings provide important insights for the design and evaluation of future high-fluence free-electron laser experiments and contribute to the understanding of non-linear electron dynamics in x-ray absorption processes in solids at the femtosecond timescale

Photon shot-noise limited transient absorption soft X-ray spectroscopy at the European XFEL

Femtosecond transient soft X-ray Absorption Spectroscopy (XAS) is a very promising technique that can be employed at X-ray Free Electron Lasers (FELs) to investigate out-of-equilibrium dynamics for material and energy research. Here we present a dedicated setup for soft X-rays available at the Spectroscopy & Coherent Scattering (SCS) instrument at the European X-ray Free Electron Laser (EuXFEL). It consists of a beam-splitting off-axis zone plate (BOZ) used in transmission to create three copies of the incoming beam, which are used to measure the transmitted intensity through the excited and unexcited sample, as well as to monitor the incoming intensity. Since these three intensity signals are detected shot-by-shot and simultaneously, this setup allows normalized shot-by-shot analysis of the transmission. For photon detection, the DSSC imaging detector, which is capable of recording up to 800 images at 4.5 MHz frame rate during the FEL burst, is employed and allows approaching the photon shot-noise limit. We review the setup and its capabilities, as well as the online and offline analysis tools provided to users

Photon shot-noise limited transient absorption soft X-ray spectroscopy at the European XFEL

Femtosecond transient soft X-ray Absorption Spectroscopy (XAS) is a very promising technique that can be employed at X-ray Free Electron Lasers (FELs) to investigate out-of-equilibrium dynamics for material and energy research. Here we present a dedicated setup for soft X-rays available at the Spectroscopy & Coherent Scattering (SCS) instrument at the European X-ray Free Electron Laser (EuXFEL). It consists of a beam-splitting off-axis zone plate (BOZ) used in transmission to create three copies of the incoming beam, which are used to measure the transmitted intensity through the excited and unexcited sample, as well as to monitor the incoming intensity. Since these three intensity signals are detected shot-by-shot and simultaneously, this setup allows normalized shot-by-shot analysis of the transmission. For photon detection, the DSSC imaging detector, which is capable of recording up to 800 images at 4.5 MHz frame rate during the FEL burst, is employed and allows approaching the photon shot-noise limit. We review the setup and its capabilities, as well as the online and offline analysis tools provided to users.Comment: 11 figure