Valence and magnetic ordering in intermediate valence compounds : TmSe versus SmB6

The intermediate valent systems TmSe and SmB6 have been investigated up to 16 and 18 GPa by ac microcalorimetry with a pressure (p) tuning realized in situ at low temperature. For TmSe, the transition from an antiferromagnetic insulator for p<3 GPa to an antiferromagnetic metal at higher pressure has been confirmed. A drastic change in the p variation of the Neel temperature (Tn) is observed at 3 GPa. In the metallic phase (p>3 GPa), Tn is found to increase linearly with p. A similar linear p increase of Tn is observed for the quasitrivalent compound TmS which is at ambiant pressure equivalent to TmSe at p=7 GPa. In the case of SmB6 long range magnetism has been detected above p=8 GPa, i.e. at a pressure slightly higher than the pressure of the insulator to metal transition. However a homogeneous magnetic phase occurs only above 10 GPa. The magnetic and electronic properties are related to the renormalization of the 4f wavefunction either to the divalent or the trivalent configurations. As observed in SmS, long range magnetism in SmB6 occurs already far below the pressure where a trivalent Sm3+ state will be reached. It seems possible, to describe roughly the physical properties of the intermediate valence equilibrium by assuming formulas for the Kondo lattice temperature depending on the valence configuration. Comparison is also made with the appearance of long range magnetism in cerium and ytterbium heavy fermion compounds.Comment: 22 pages including figure

Multiconfigurational nature of 5f orbitals in uranium and plutonium intermetallics

Uranium and plutonium's 5f electrons are tenuously poised between strongly bonding with ligand spd-states and residing close to the nucleus. The unusual properties of these elements and their compounds (eg. the six different allotropes of elemental plutonium) are widely believed to depend on the related attributes of f-orbital occupancy and delocalization, for which a quantitative measure is lacking. By employing resonant x-ray emission spectroscopy (RXES) and x-ray absorption near-edge structure (XANES) spectroscopy and making comparisons to specific heat measurements, we demonstrate the presence of multiconfigurational f-orbital states in the actinide elements U and Pu, and in a wide range of uranium and plutonium intermetallic compounds. These results provide a robust experimental basis for a new framework for understanding the strongly-correlated behavior of actinide materials.Comment: 30 pages, concatenated article and supporting information, 10 figure

Evidence for suppressed metallicity on the surface of La2-xSrxCuO4 and Nd2-xCexCuO4

Hard X-ray Photoemission spectroscopy (PES) of copper core electronic states, with a probing depth of $\sim$60 \AA, is used to show that the Zhang-Rice singlet feature is present in La$_2$CuO$_4$ but is absent in Nd$_2$CuO$_4$. Hole- and electron doping in La$_{2-x}$Sr$_x$CuO$_4$ (LSCO) and Nd$_{2-x}$Ce$_x$CuO$_4$ (NCCO) result in new well-screened features which are missing in soft X-ray PES. Impurity Anderson model calculations establish metallic screening as its origin, which is strongly suppressed within 15 $\text{\AA}$ of the surface. Complemented with X-ray absorption spectroscopy, the small chemical-potential shift in core levels ($\sim0.2$ eV) are shown to be consistent with modifications of valence and conduction band states spanning the band gap ($\sim1$ eV) upon hole- and electron-doping in LSCO and NCCO.Comment: 4 pages, 4 figure

A determination of the pairing interaction in the high Tc cuprate superconductor Tl2Ba2CaCu2O8 (Tl2212)

We have measured the near-normal reflectance of Tl2Ba2CaCu2O8 (Tl2212) for energies from 0.1 to 4.0 eV at room temperature and used a Kramers-Kronig analysis to find the complex, frequency dependent dielectric function, from which the optical conductivity was determined. Using Thermal-Difference-Reflectance (TDR) Spectroscopy the reflectance of the sample in the normal state just above the superconducting transition, and in the superconducting state were then obtained. From these data we determined the ratio of the superconducting- to normal-state optical conductivities. Mattis and Bardeen had calculated this function within the BCS theory, where the gap is a fixed energy-independent quantity. Taking into account the retarded nature of the electron-phonon coupling results in a complex, energy dependent gap causing deviations from the Mattis-Bardeen plot at energies where the phonon coupling function is large. We find a typical deviation near the phonon energies in Tl2212, and in addition, at 1.2 and 1.7eV. The phonon, and these electronic terms can each be described by a coupling constant. None of which by itself gives rise to a high transition temperature, but the combination does. Using Resonant Inelastic X-Ray Scattering (RIXS) we find that the d-to-d excitations of the cuprate ion in Tl2212 fall at the same energies as the dips in the Mattis-Bardeen plot. We conclude that the high superconducting transition temperature of the cuprates is due to the sum of the phonon interaction, and interactions with the Cu-ion d-shell.Comment: Preprint submitted to Physica C. Paper presented at M2S-HTSC-VIII, Dresden, Germany, July 9-14,200

Magnetic anisotropy at the buried CoO/Fe interface

Interfaces between antiferromagnetic CoO and ferromagnetic Fe are typically characterized by the development of Fe oxides. Recently, it was shown that the use of a proper ultra-thin Co buffer layer prevents the formation of Fe oxides [Brambilla et al., Appl. Surf. Sci. 362, 374 (2016)]. In the present work, we investigate the magnetic properties of such an interface, and we find evidence for an in-plane uniaxial magnetic anisotropy, which is characterized by a multijump reversal behavior in the magnetization hysteresis loops. X-ray photoemission spectroscopy and element-sensitive hysteresis loops reveal that the occurrence of such an anisotropy is a phenomenon developing at the very interface

Strain induced phase separation in La0.7Sr0.3MnO3 thin films.

La0.7Sr0.3MnO3 thin films having different thicknesses were grown by pulsed laser deposition with in situ reflection high energy electron diffraction diagnostics on LaAlO3 substrates. The mismatch between film and substrate gives rise to an in-plane compressive biaxial strain, which partially relaxes in films thicker than 30 unit cells. Accordingly, the ratio between the out-of-plane and the in-plane lattice parameter c/a varies between 1.06 fully strained and 1.03 partially relaxed. In-plane compressive strain favors the stabilization of the 3z2−r2 orbitals chain-type antiferromagnetic phase, thus giving rise to a sizeable x-ray absorption linear dichroism signal. The shape of the linear dichroism depends weakly on the c/a ratio, while its intensity strongly increases with c/a. At the same time, the metal-insulator transition temperature shifts from about 360 K towards lower temperatures with decreasing thickness, eventually reaching an insulating state for the 30 unit cells film. Low-temperature nuclear magnetic resonance spectra show a decrease of the MnDE doubleexchange metallic contribution with decreasing the thickness, which becomes negligible in the 30 unit cells thick film. The experimental results demonstrate a strain driven competition between two stable phases: the orbital ordered chain-type insulating antiferromagnetic and the orbital disordered metallic ferromagnetic. For intermediate values of the epitaxial strain the local minimum state of the system lies in a gap region between the two stable phases. Such a region has glassy characteristics with coexisting clusters of the two phases. The strain is used as a driving force to span the glassy region

Coherent phonons and the interplay between charge density wave and Mott phases in 1TT-TaSe2_{2}

1$T$-TaSe$_{2}$ is host to coexisting strongly-correlated phases including charge density waves (CDWs) and an unusual Mott transition at low temperature. Here, we investigate coherent phonon oscillations in 1$T$-TaSe$_{2}$ using a combination of time- and angle-resolved photoemission spectroscopy (TR-ARPES) and time-resolved reflectivity (TRR). Perturbation by a femtosecond laser pulse triggers a modulation of the valence band binding energy at the $\Gamma$-point, related to the Mott gap, that is consistent with the in-plane CDW amplitude mode frequency. By contrast, TRR measurements show a modulation of the differential reflectivity comprised of multiple frequencies belonging to the distorted CDW lattice modes. Comparison of the temperature dependence of coherent and spontaneous phonons across the CDW transition shows that the amplitude mode intensity is more easily suppressed during perturbation of the CDW state by the optical excitation compared to other modes. Our results clearly identify the relationship of the in-plane CDW amplitude mode with the Mott phase in 1$T$-TaSe$_{2}$ and highlight the importance of lattice degrees of freedom.Comment: 7 pages, 4 figures, supplemental materia

Structural, Electronic and Magnetic Properties of a Few Nanometer-Thick Superconducting NdBa₂Cu₃O₇ Films

Abstract: Epitaxial films of high critical temperature (Tc) cuprate superconductors preserve their transport properties even when their thickness is reduced to a few nanometers. However, when approaching the single crystalline unit cell (u.c.) of thickness, Tc decreases and eventually, superconductivity is lost. Strain originating from the mismatch with the substrate, electronic reconstruction at the interface and alteration of the chemical composition and of doping can be the cause of such changes. Here, we use resonant inelastic x-ray scattering at the Cu L3 edge to study the crystal field and spin excitations of NdBa2Cu3O7x ultrathin films grown on SrTiO3, comparing 1, 2 and 80 u.c.-thick samples. We find that even at extremely low thicknesses, the strength of the in-plane superexchange interaction is mostly preserved, with just a slight decrease in the 1 u.c. with respect to the 80 u.c.-thick sample. We also observe spectroscopic signatures for a decrease of the hole-doping at low thickness, consistent with the expansion of the c-axis lattice parameter and oxygen deficiency in the chains of the first unit cell, determined by high-resolution transmission microscopy and x-ray diffraction