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Register a new userElectronic structures of UX$_3$ (X=Al, Ga, and In) studied by photoelectron spectroscopy
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The electronic structures of UX$_3$ (X=Al, Ga, and In) were studied by photoelectron spectroscopy to understand the relationship between their electronic structures and magnetic properties. The band structures and Fermi surfaces of UAl$_3$ and UGa$_3$ were revealed experimentally by angle-resolved photoelectron spectroscopy (ARPES), and they were compared with the result of band-structure calculations. The topologies of the Fermi surfaces and the band structures of UAl$_3$ and UGa$_3$ were explained reasonably well by the calculation, although bands near the Fermi level ($E_mathrm{F}$) were renormalized owing to the finite electron correlation effect. The topologies of the Fermi surfaces of UAl$_3$ and UGa$_3$ are very similar to each other, except for some minor differences. Such minor differences in their Fermi surface or electron correlation effect might take an essential role in their different magnetic properties. No significant changes were observed between the ARPES spectra of UGa$_3$ in the paramagnetic and antiferromagnetic phases, suggesting that UGa$_3$ is an itinerant weak antiferromagnet. The effect of chemical pressure on the electronic structures of UX$_3$ compounds was also studied by utilizing the smaller lattice constants of UAl$_3$ and UGa$_3$ than that of UIn$_3$. The valence band spectrum of UIn$_3$ is accompanied by a satellite-like structure on the high-binding-energy side. The core-level spectrum of UIn$_3$ is also qualitatively different from those of UAl$_3$ and UGa$_3$. These findings suggest that the U~$5f$ states in UIn$_3$ are more localized than those in UAl$_3$ and UGa$_3$.
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The electronic structure of the unconventional superconductor UTe$_2$ was studied by resonant photoelectron spectroscopy (RPES) and angle-resolved photoelectron spectroscopy (ARPES) with soft X-ray synchrotron radiation. The partial $mathrm{U}~5f$ density of states of UTe$_2$ were imaged by the $mathrm{U}~4d$--$5f$ RPES and it was found that the $mathrm{U}~5f$ state has an itinerant character, but there exists an incoherent peak due to the strong electron correlation effects. Furthermore, an anomalous admixture of the $mathrm{U}~5f$ states into the $mathrm{Te}~5p$ bands was observed at a higher binding energy, which cannot be explained by band structure calculations. On the other hand, the band structure of UTe$_2$ was obtained by ARPES and its overall band structure were mostly explained by band structure calculations. These results suggest that the $mathrm{U}~5f$ states of UTe$_2$ have itinerant but strongly-correlated nature with enhanced hybridization with the $mathrm{Te}~5p$ states.
Soft and hard X-ray photoelectron spectroscopy (PES) has been performed for one of the heavy fermion system CeRu$_2$Si$_2$ and a $4f$-localized ferromagnet CeRu$_2$Ge$_2$ in the paramagnetic phase. The three-dimensional band structures and Fermi surface (FS) shapes of CeRu$_2$Si$_2$ have been determined by soft X-ray $h u$-dependent angle resolved photoelectron spectroscopy (ARPES). The differences in the Fermi surface topology and the non-$4f$ electronic structures between CeRu$_2$Si$_2$ and CeRu$_2$Ge$_2$ are qualitatively explained by the band-structure calculation for both $4f$ itinerant and localized models, respectively. The Ce valences in CeRu$_2X_2$ ($X$ = Si, Ge) at 20 K are quantitatively estimated by the single impurity Anderson model calculation, where the Ce 3d hard X-ray core-level PES and Ce 3d X-ray absorption spectra have shown stronger hybridization and signature for the partial $4f$ contribution to the conduction electrons in CeRu$_2$Si$_2$.
The electronic structures of the ferromagnetic superconductors $mathrm{UGe}_2$ and $mathrm{UCoGe}$ in the paramagnetic phase were studied by angle-resolved photoelectron spectroscopy using soft X-rays ($h u =400-500$). The quasi-particle bands with large contributions from $mathrm{U}~5f$ states were observed in the vicinity of $E_mathrm{F}$, suggesting that the $mathrm{U}~5f$ electrons of these compounds have an itinerant character. Their overall band structures were explained by the band-structure calculations treating all the $mathrm{U}~5f$ electrons as being itinerant. Meanwhile, the states in the vicinity of $E_mathrm{F}$ show considerable deviations from the results of band-structure calculations, suggesting that the shapes of Fermi surface of these compounds are qualitatively different from the calculations, possibly caused by electron correlation effect in the complicated band structures of the low-symmetry crystals. Strong hybridization between $mathrm{U}~5f$ and $mathrm{Co}~3d$ states in $mathrm{UCoGe}$ were found by the $mathrm{Co}~2p-3d$ resonant photoemission experiment, suggesting that $mathrm{Co}~3d$ states have finite contributions to the magnetic, transport, and superconducting properties.
High-energy-resolution core-level and valence-band photoelectron spectroscopic studies were performed for the heavy Fermion uranium compounds UGe2, UCoGe, URhGe, URu2Si2, UNi2Al3, UPd2Al3, and UPt3 as well as typical localized and itinerant uranium compounds to understand the relationship between the uranium valence state and their core-level spectral line shapes. In addition to the main line and high-binding energy satellite structure recognized in the core-level spectra of uranium compounds, a shoulder structure on the lower binding energy side of the main lines of localized and nearly localized uranium compounds was also found. The spectral line shapes show a systematic variation depending on the U 5f electronic structure. The core-level spectra of UGe2, UCoGe, URhGe, URu2Si2, and UNi2Al3 are rather similar to those of itinerant compounds, suggesting that U 5f electrons in these compounds are well hybridized with ligand states. On the other hand, the core-level spectra of UPd2Al3 and UPt3 show considerably different spectral line shapes from those of the itinerant compounds, suggesting that U 5f electrons in UPd2Al3 and UPt3 are less hybridized with ligand states, leading to the correlated nature of U 5f electrons in these compounds. The dominant final state characters in their core-level spectra suggest that the numbers of 5f electrons in UGe2, UCoGe, URhGe, URu2Si2, UNi2Al3, and UPd2Al3 are close to but less than three, while that of UPt3 is close to two rather than to three.
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.
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