121 research outputs found
Bulk electronic structure of non-centrosymmetric EuTGe3 (T= Co, Ni, Rh, Ir) studied by hard x-ray photoelectron spectroscopy
Non-centrosymmetric EuTGe3 (T=Co, Ni, Rh, and Ir) possesses magnetic Eu2+
ions and antiferromagnetic ordering appears at low temperatures. Transition
metal substitution leads to changes of the unit cell volume and of the magnetic
ordering. However, the magnetic ordering temperature does not scale with the
volume change and the Eu valence is expected to remain divalent. Here we study
the bulk electronic structure of non-centrosymmetric EuTGe3 (T=Co, Ni, Rh, and
Ir) by hard x-ray photoelectron spectroscopy. The Eu 3d core level spectrum
confirms the robust Eu2+ valence state against the transition metal
substitution with a small contribution from Eu3+. The estimated Eu mean-valence
is around 2.1 in these compounds as confirmed by multiplet calculations. In
contrast, the Ge 2p spectrum shifts to higher binding energy upon changing the
transition metal from 3d to 4d to 5d elements, hinting of a change in the Ge-T
bonding strength. The valence bands of the different compounds are found to be
well reproduced by ab initio band structure calculations
Valence Instability of YbCuSi through its quantum critical point
We report Resonant inelastic x-ray scattering measurements (RIXS) in
YbCuSi at the Yb L edge under high pressure (up to 22 GPa) and at
low temperatures (down to 7 K) with emphasis on the vicinity of the transition
to a magnetic ordered state. We find a continuous valence change towards the
trivalent state with increasing pressure but with a pronounced change of slope
close to the critical pressure. Even at 22 GPa the Yb state is not fully
achieved. The pressure where this feature is observed decreases as the
temperature is reduced to 9 GPa at 7K, a value close to the critical pressure
(\itshape{p\normalfont{}}\normalfont 7.5 GPa) where magnetic
order occurs. The decrease in the valence with decreasing temperature
previously reported at ambient pressure is confirmed and is found to be
enhanced at higher pressures. We also compare the f electron occupancy between
YbCuSi and its Ce-counterpart, CeCuSi
Metal-ligand interplay in strongly-correlated oxides: a parametrized phase diagram for pressure induced spin transitions
We investigate the magnetic properties of archetypal transition-metal oxides
MnO, FeO, CoO and NiO under very high pressure by x-ray emission spectroscopy
at the K\beta line. We observe a strong modification of the magnetism in the
megabar range in all the samples except NiO. The results are analyzed within a
multiplet approach including charge-transfer effects. The pressure dependence
of the emission line is well accounted for by changes of the ligand field
acting on the d electrons and allows us to extract parameters like local
d-hybridization strength, O-2p bandwidth and ionic crystal field across the
magnetic transition. This approach allows a first-hand insight into the
mechanism of the pressure induced spin transition.Comment: 5 pages, 3 figure
Charge distribution across capped and uncapped infinite-layer neodymium nickelate thin films
Charge ordering (CO) phenomena have been widely debated in
strongly-correlated electron systems mainly regarding their role in
high-temperature superconductivity. Here, we elucidate the structural and
charge distribution in NdNiO thin films prepared with and without capping
layers, and characterized by the absence and presence of CO. Our
microstructural and spectroscopic analysis was done by scanning transmission
electron microscopy-electron energy loss spectroscopy (STEM-EELS) and hard
x-ray photoemission spectroscopy (HAXPES). Capped samples show Ni, with
an out-of-plane (o-o-p) lattice parameter of around 3.30 angstroms indicating
good stabilization of the infinite-layer structure. Bulk-sensitive HAXPES on
Ni-2p shows weak satellite feature indicating large charge-transfer energy. The
uncapped samples evidence an increase of the o-o-p parameter up to 3.65
angstroms on the thin-film top, and spectroscopies show signatures of higher
valence in this region (towards Ni). Here, 4D-STEM demonstrates (3,0,3)
oriented stripes which emerge from partially occupied apical oxygen. Those
stripes form quasi-2D coherent domains viewed as rods in the reciprocal space
with r.l.u. extension located at Q = () r.l.u. and Q = () r.l.u. The stripes associated with oxygen re-intercalation
concomitant with hole doping suggests a possible link to the previously
reported CO in infinite-layer nickelate thin films
Temperature and pressure-induced spin-state transitions in LaCoO3
We report the continuous variation of the spin moment of cobalt in LaCoO3
across its temperature and pressure-induced spin transitions evidenced with
K\beta emission spectra. The first thermal transition is best described by a
transition to an orbitally nondegenerate intermediate spin (S=1) state. In
parallel, continuous redistribution of the 3d electrons is also indicated by
partial fluorescence yield X-ray absorption spectra. At high pressure, our
study confirms that the material becomes low spin between 40 and 70 kbar at
room temperature
a tool to disentangle overlapping core-excited states
We have measured resonant-Auger decay following Cl 1s−1 excitations in HCl and
CH3Cl molecules, and extracted the pseudo-cross sections of different Cl 2p−2
final states. These cross sections show clear evidence of shake processes as
well as contributions of electronic state-lifetime interference (ELI). To
describe the spectra we developed a fit approach that takes into account ELI
contributions and ultrafast nuclear dynamics in dissociative core-excited
states. Using this approach we utilized the ELI contributions to obtain the
intensity ratios of the overlapping states Cl 1s−14pπ/1s−14pσ in HCl and Cl
1s−14pe/1s−14pa1 in CH3Cl. The experimental value for HCl is compared with
theoretical results showing satisfactory agreement
Oxygen impurities link bistability and magnetoresistance in organic spin valves
Vertical cross-bar devices based on manganite and cobalt injecting electrodes and metal-quinoline molecular transport layer are known to manifest both magnetoresistance and electrical bistability. The two effects are strongly interwoven, inspiring new device applications such as electrical control of the magnetoresistance and magnetic modulation of bistability. To investigate the full device functionality, we first identify the mechanism responsible for electrical switching by associating the electrical conductivity and the impedance behavior with chemical states of buried layers obtained by in operando photoelectron spectroscopy. These measurements revealed that a significant fraction of oxygen ions migrates under voltage polarity, resulting in a modification of the electronic properties of the organic material and of the oxidation of interfacial layer with ferromagnetic contacts. Variable oxygen doping of the organic molecule represents the key element for correlating bistability and magnetoresistance and our measurements provide the first experimental evidence in favor of the impurity band model describing the spin transport in organic semiconductors in similar devices
- …