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Register a new userSynchrotron x-ray spectroscopy studies of valence and magnetic state in europium metal to extreme pressures
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In order to probe the changes in the valence state and magnetic properties of Eu metal under extreme pressure, x-ray absorption near-edge spectroscopy, x-ray magnetic circular dichroism and synchrotron Mossbauer spectroscopy experiments have been carried out. The Mossbauer isomer shift exhibits an anomalous pressure dependence, passing through a maximum near 20 GPa. Density functional theory has been applied to give insight into the pressure-induced changes in both Eus electronic structure and Mossbauer isomer shift. Contrary to previous reports, Eu is found to remain nearly divalent to the highest pressures reached (87 GPa) with magnetic order persisting to at least 50 GPa. These results should lead to a better understanding of the nature of the superconducting state found above 75 GPa and of the sequence of structural phase transitions observed to 92 GPa.
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X-ray magnetic circular dichroism (XMCD) at the Eu L-edge (2p->5d) in two compounds exhibiting valence fluctuation, namely EuNi2(Si0.18Ge0.82)2 and EuNi2P2, has been investigated at pulsed high magnetic fields of up to 40 T. A distinct XMCD peak corresponding to the trivalent state (Eu3+; f6), whose ground state is nonmagnetic (J=0), was observed in addition to the main XMCD peak corresponding to the magnetic (J=7/2) divalent state (Eu2+; f7). This result indicates that the 5d electrons belonging to both valence states are magnetically polarized. It was also found that the ratio P5d(3+)/P5d(2+) between the polarization of 5d electrons (P5d) in the Eu3+ state and that of Eu2+ is ~ 0.1 in EuNi2(Si0.18Ge0.82)2 and ~ 0.3 in EuNi2P2 at magnetic fields where their macroscopic magnetization values are the same. The possible origin of the XMCD of the Eu3+ state and an explanation of the dependence of P5d(3+)/P5d(2+) on the material are discussed in terms of hybridization between the conduction electrons and the f electrons.
The valence state of Yb ions in beta-YbAlB4 and its polymorph alpha-YbAlB4 has been investigated by using X-ray absorption and emission spectroscopy in SPring-8 at temperatures from 2 to 280 K. The observed Yb valence is 2.78 +- 0.01 in beta-YbAlB4 at 2 K by using the X-ray emission spectroscopy. The valence is found to gradually increase with increasing temperature toward the trivalent state, and the characteristic temperature of the valence fluctuation is expected to be about 290 K. We also found a small increase in the Yb valence (~0.002) by applying a magnetic field of 32 T at 40 K to beta-YbAlB4.
The pressure-dependent relation between Eu valence and lattice structure in model compound EuO is studied with synchrotron-based x-ray spectroscopic and diffraction techniques. Contrary to expectation, a 7% volume collapse at $approx$ 45 GPa is accompanied by a reentrant Eu valence transition into a $emph{lower}$ valence state. In addition to highlighting the need for probing both structure and electronic states directly when valence information is sought in mixed-valent systems, the results also show that widely used bond-valence methods fail to quantitatively describe the complex electronic valence behavior of EuO under pressure.
We investigate LiVS2 and LiVSe2 with a triangular lattice as itinerant analogues of LiVO2, known for the formation of valence bond solid (VBS) state out of S = 1 frustrated magnet. LiVS2, which is located at the border between a metal and a correlated insulator, shows a first ordered transition from a paramagnetic metal to a VBS insulator at Tc ~ 305 K upon cooling. The presence of VBS state in the close vicinity of insulator-metal transition may suggest the importance of itinerancy in the formation of VBS state. We argue that the high temperature metallic phase of LiVS2 has a pseudo-gap, likely originating from the VBS fluctuation. LiVSe2 was found to be a paramagnetic metal down to 2 K.
The compound, Sr3NiPtO6, belonging to a K4CdCl6-type rhombohedral structure, has been reported not to exhibit magnetic ordering at least down to 1.8 K, despite a relatively large value of paramagnetic Curie temperature. This is attributable to geometrical frustration. Here we report the results of our efforts to gradually replace Sr by Ba and to probe the influence of positive (external) and negative (chemical) pressure on the magnetic behavior of this compound. In the Ba substituted series, single phase is formed up to x= 1.0 with Ba substituting for Sr. The magnetic properties of the parent compound in the entire temperature range of investigation are not influenced at all in any of the compositions studied as well as under external pressure (investigated up to 10 kbar). Spin-liquid-like heat-capacity behavior (finite linear term) is observed even in Ba substituted specimens. Thus, the magnetic anomalies of this compound are quite robust.
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