Nonpareil Yb behavior in YbMn6Ge(6-x)Sn(x).

We investigate the temperature dependence of the Yb valence in YbMn6Ge1.8Sn4.2 and YbMn6Ge1.6Sn4.4 using resonant inelastic x-ray scattering experiments. Yb is found to be in an intermediate valent state in the whole investigated temperature range (10-450 K). We thus prove that the unusually high magnetic ordering temperature of Yb (∼60 and 90 K for x=4.2 and 4.4, respectively) involves an intermediate valent Yb, an unprecedentedly observed phenomenon. Further, an anomalous increase in the Yb valence is observed upon cooling. A scenario is proposed to explain this unusual behavior. It is based on the presence of magnetically ordered Mn moments and on an Anderson Hamiltonian with a Zeeman term modeling the magnetic interactions.

Ultrafast spin-polarized electron dynamics in the unoccupied topological surface state of Bi2Se3.

The three-dimensional topological insulator Bi2Se3 presents two cone-like dispersive topological surface states centered at the [Formula: see text] point. One of them is unoccupied in equilibrium conditions and located 1.8 eV above the other one lying close to the Fermi level. In this work we employ time- and angle-resolved photoemission spectroscopy with circularly polarized pump photons to selectively track the spin dynamics of the empty topological states. We observe that spin-polarized electrons flow along the topological cone and recombine towards the unpolarized bulk states on a timescale of few tens of femtoseconds. This provides direct evidence of the capability to trigger a spin current with circularly polarized light.

A flexible experimental setup for femtosecond time-resolved broad-band ellipsometry and magneto-optics.

A versatile experimental setup for femtosecond time-resolved ellipsometry and magneto-optical Kerr effect measurements in the visible light range is described. The apparatus is based on the pump-probe technique and combines a broad-band probing beam with an intense near-infrared pump. According to Fresnel scattering matrix formalism, the analysis of the reflected beam at different polarization states of the incident probe light allows one to determine the diagonal and the off-diagonal elements of the dielectric tensor in the investigated sample. Moreover, the pump-probe method permits to study the dynamics of the dielectric response after a short and intense optical excitation. The performance of the experimental apparatus is tested on CrO2 single crystals as a benchmark.

Coherent ultrafast spin-dynamics probed in three dimensional topological insulators.

Topological insulators are candidates to open up a novel route in spin based electronics. Different to traditional ferromagnetic materials, where the carrier spin-polarization and magnetization are based on the exchange interaction, the spin properties in topological insulators are based on the coupling of spin- and orbit interaction connected to its momentum. Specific ways to control the spin-polarization with light have been demonstrated: the energy momentum landscape of the Dirac cone provides spin-momentum locking of the charge current and its spin. We investigate a spin-related signal present only during the laser excitation studying real and imaginary part of the complex Kerr angle by disentangling spin and lattice contributions. This coherent signal is only present at the time of the pump-pulses' light field and can be described in terms of a Raman coherence time. The Raman transition involves states at the bottom edge of the conduction band. We demonstrate a coherent femtosecond control of spin-polarization for electronic states at around the Dirac cone.

An innovative Yb-based ultrafast deep ultraviolet source for time-resolved photoemission experiments.

Time- and angle-resolved photoemission spectroscopy is a powerful technique to study ultrafast electronic dynamics in solids. Here, an innovative optical setup based on a 100-kHz Yb laser source is presented. Exploiting non-collinear optical parametric amplification and sum-frequency generation, ultrashort pump (hν = 1.82 eV) and ultraviolet probe (hν = 6.05 eV) pulses are generated. Overall temporal and instrumental energy resolutions of, respectively, 85 fs and 50 meV are obtained. Time- and angle-resolved measurements on BiTeI semiconductor are presented to show the capabilities of the setup.

BaVS3 probed by V L edge x-ray absorption spectroscopy.

Polarization dependent vanadium L edge x-ray absorption spectra of BaVS(3) single crystals are measured in the four phases of the compound. The difference between signals with the polarizations E perpendicular to c and E is parallel to c (linear dichroism) changes with temperature. Besides increasing the intensity of one of the maxima, a new structure appears in the pre-edge region below the metal-insulator transition. More careful examination brings to light that the changes start already with pretransitional charge density wave fluctuations. Simple symmetry analysis suggests that the effect is related to rearrangements in the E(g) and A(1g) states, and is compatible with the formation of four inequivalent V-sites along the V-S chain.

A versatile apparatus for time-resolved photoemission spectroscopy via femtosecond pump-probe experiments.

A laser-based system for time-resolved photoemission spectroscopy using up to 6.2 eV photons is presented. The versatility of the laser source permits several combinations of pump and probe photon energies with pulse durations of 50-100 fs. The ultrahigh vacuum system, equipped with evaporators, a low energy electron diffraction system and an Auger spectrometer, grants the possibility to grow and characterize thin films in situ. The electron energy analyzer is a time-of-flight spectrometer with a multianode detector allowing high count rates. The performance of the whole experimental setup is investigated on Cu(100), Cu(111), and Ag(111) single crystals.

Observation of two nondispersive magnetic excitations in NiO by resonant inelastic soft-X-Ray scattering.

We present high resolution (DeltaE=120 meV) resonant inelastic x-ray scattering data measured at the Ni L3 edge (2p_{3/2}-->3d) on the paradigmatic antiferromagnetic oxide NiO. Spectra reveal clear signatures of magnetic excitations at approximately 95 and approximately 190 meV whose energy seems independent from transferred momentum. These spectral features are well reproduced by a single Ni2+ ion model in an effective exchange field. Within this local model the two magnetic excitations are characterized by a variation of the atomic magnetic moment along the local ordering direction (DeltaS_{alpha}) of one and two units. The DeltaS_{alpha}=2 case has different nature from bimagnons observed in optical Raman spectra, for which DeltaS_{alpha}=0.

Using high energy angle resolved photoelectron spectroscopy to reveal the charge density in solids.

The charge density in solids is a fundamental parameter. Here we demonstrate that the charge density can be determined by the use of angle resolved photoelectron spectroscopy. The method, which involves a Fourier-like transform from momentum space to real space, is demonstrated by utilizing soft x-ray angle resolved photoelectron spectroscopy to sample the complete three-dimensional Brillouin zone of copper. It is also shown that this can be done in an energy resolved way as to extract the charge density contribution from states of a particular energy.

Localized electronic excitations in NiO studied with resonant inelastic X-Ray scattering at the Ni M threshold: evidence of spin flip.

We studied the neutral electronic excitations of NiO localized at the Ni sites by measuring the resonant inelastic x-ray scattering (RIXS) spectra at the Ni M2,3 edges. The good energy resolution allows an unambiguous identification of several spectral features due to excitations. The dependence of the RIXS spectra on the excitation energy gives evidence of local spin flip and yields a value of 125 +/- 15 meV for the antiferromagnetic exchange interaction. Accurate crystal field parameters are also obtained.

Angle resolved photoemission from Nd1.85Ce0.15CuO4 using high energy photons: a fermi surface investigation.

We have performed an angle resolved photoemission study on a single crystal of the optimally electron doped (n-type) cuprate superconductor Nd2-xCexCuO4 (x=0.15) at a photon energy of 400 eV. The Fermi surface is mapped out and is, in agreement with earlier measurements, of hole-type with the expected Luttinger volume. However, comparing with previous low energy measurements, we observe a different Fermi surface shape and a different distribution of spectral intensity around the Fermi surface contour. The observed Fermi surface shape indicates a stronger electron correlation in the bulk as compared to the surface.

New spectroscopy solves an old puzzle: the Kondo scale in heavy fermions.

Resonant inelastic x-ray scattering (RIXS) yields clear evidence of spectroscopic Kondo scales in heavy fermions. In YbInCu4 and YbAgCu4 RIXS probes the Yb2+ component of the hybrid ground state and the temperature dependence of the Yb 4f occupation. We report a sudden valence change at a phase transition in YbInCu4, but a continuous temperature dependence in YbAgCu4, consistent with the predictions of the Anderson impurity model, for a Kondo temperature T(K) = 70 K. These results solve a long-standing controversy and establish RIXS as a quantitative probe of the electronic structure of strongly correlated electron systems.

Soft X-ray Emission Spectroscopy at ESRF Beamline 26 Based on a Helical Undulator.

A new soft X-ray spectrograph for X-ray emission spectroscopy excited by synchrotron radiation is presented. The apparatus is now installed on beamline 26 at the ESRF in Grenoble. A brief description of the beamline is given and then several components of the spectrograph are covered in more detail. Results of experiments performed both with direct non-monochromated undulator radiation and with monochromated radiation are reported.

First-principles theory of intermediate-valence f-electron systems.

We propose a first-principles based method for calculating the electronic structure and total energy of solids in an intermediate-valence configuration. The method takes into account correlation effects (d-f Coulomb interaction) and many-body renormalization of the effective hybridization parameter of the f system. As an example, the formation of a pressure-induced intermediate-valence state in Yb is considered and its electronic structure and equation of state are calculated and compared to experimental data. The agreement is found to be excellent for both properties, and we argue that the developed method, which applies to any element or compound, provides for the first time a quantitative theoretical treatment of intermediate-valence materials.

Low energy electronic excitations in the layered cuprates studied by copper L3 resonant inelastic x-ray scattering.

We have measured the resonant inelastic x-ray scattering (RIXS) spectra at the Cu L3 edge in a variety of cuprates. Exploiting a considerably improved energy resolution (0.8 eV) we recorded significant dependencies on the sample composition and orientation, on the scattering geometry, and on the incident photon polarization. The RIXS final states correspond to two families of electronic excitations, having local (dd excitations) and nonlocal (charge-transfer) character. The dd energy splitting can be estimated with a simple crystal field model. The RIXS at the L3 edge demonstrates here a great potential, thanks to the resonance strength and to the large 2p spin-orbit splitting.