Reentrant valence transition in EuO at high pressures: beyond the bond-valence model

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.Comment: 5 pages, 4 figure

Effect of Cr spacer on structural and magnetic properties of Fe/Gd multilayers

In this work we analyse the role of a thin Cr spacer between Fe and Gd layers on structure and magnetic properties of a [Fe(35A)/Cr(tCr)/Gd(50A)/Cr(tCr)]x12 superlattice. Samples without the Cr spacer (tCr=0) and with a thin tCr=4A are investigated using X-ray diffraction, polarized neutron and resonance X-ray magnetic reflectometry, SQUID magnetometery, magneto-optical Kerr effect and ferromagnetic resonance techniques. Magnetic properties are studied experimentally in a wide temperature range 4-300K and analysed theoretically using numerical simulation on the basis of the mean-field model. We show that a reasonable agreement with the experimental data can be obtained considering temperature dependence of the effective field parameter in gadolinium layers. The analysis of the experimental data shows that besides a strong reduction of the antiferromagnetic coupling between Fe and Gd, the introduction of Cr spacers into Fe/Gd superlattice leads to modification of both structural and magnetic characteristics of the ferromagnetic layers

Theory of Room Temperature Ferromagnet V(TCNE)_x (1.5 < x < 2): Role of Hidden Flat Bands

Theoretical studies on the possible origin of room temperature ferromagnetism (ferromagnetic once crystallized) in the molecular transition metal complex, V(TCNE)_x (1.5<x<2) have been carried out. For this family, there have been no definite understanding of crystal structure so far because of sample quality, though the effective valence of V is known to be close to +2. Proposing a new crystal structure for the stoichiometric case of x=2, where the valence of each TCNE molecule is -1 and resistivity shows insulating behavior, exchange interaction among d-electrons on adjacent V atoms has been estimated based on the cluster with 3 vanadium atoms and one TCNE molecule. It turns out that Hund's coupling among d orbitals within the same V atoms and antiferromagnetic coupling between d oribitals and LUMO of TCNE (bridging V atoms) due to hybridization result in overall ferromagnetism (to be precise, ferrimagnetism). This view based on localized electrons is supplemented by the band picture, which indicates the existence of a flat band expected to lead to ferromagnetism as well consistent with the localized view. The off-stoichiometric cases (x<2), which still show ferromagnetism but semiconducting transport properties, have been analyzed as due to Anderson localization.Comment: Accepted for publication in J. Phys. Soc. Jpn. Vol.79 (2010), No. 3 (March issue), in press; 6 pages, 8 figure

Different Response of Transport and Magnetic Properties of BaIrO\u3csub\u3e3\u3c/sub\u3e to Chemical and Physical Pressure

A combination of x-ray absorption, x-ray-diffraction, and transport measurements at high pressure is used to investigate the interplay between the electronic properties of Ir 5d states and lattice degrees of freedom in the weakly ferromagnetic insulator BaIrO3. Although the Ir 5d local magnetic moment is highly stable against lattice compression, remaining nearly unperturbed to at least 30 GPa, the weak ferromagnetism (net ordered moment) is quickly quenched by 4.5 GPa (3% volume reduction). Under chemical pressure, where Sr is substituted for the larger Ba in BaIrO3, the local magnetic moment on Ir remains stable, but the weak ferromagnetism is quenched after only 1.7% volume reduction. The magnetic ordering temperature Tm is also more strongly suppressed by chemical pressure compared to physical pressure. In addition, under ~23−at.% Sr doping, BaIrO3 undergoes a transition to a paramagnetic metallic state. Resistivity measurements indicate that BaIrO3 remains an electrical insulator to at least 9 GPa, a much higher pressure than required to quench the weak ferromagnetism (∼4.5GPa). Such a disparate response of transport and magnetic properties to chemical and physical pressure is likely rooted in the different compression rates of the (a,c) lattice parameters with Sr doping and applied pressure and the effect of related lattice distortions on electronic bandwidth and exchange interactions in this strongly spin-orbit-coupled system

Fragility of ferromagnetic double exchange interactions and pressure tuning of magnetism in 3d-5d double perovskite Sr2FeOsO6

FAPESP - FUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULOThe ability to tune exchange (magnetic) interactions between 3d transition metals in perovskite structures has proven to be a powerful route to discovery of novel properties. Here we demonstrate that the introduction of 3d-5d exchange pathways in double perovskites enables additional tunability, a result of the large spatial extent of 5d wave functions. Using x-ray probes of magnetism and structure at high pressure, we show that compression of Sr2FeOsO6 drives an unexpected continuous change in the sign of Fe-Os exchange interactions and a transition from antiferromagnetic to ferrimagnetic order. We analyze the relevant electron-electron interactions, shedding light into fundamental differences with the more thoroughly studied 3d-3d systems.The ability to tune exchange (magnetic) interactions between 3d transition metals in perovskite structures has proven to be a powerful route to discovery of novel properties. Here we demonstrate that the introduction of 3d-5d exchange pathways in double perovskites enables additional tunability, a result of the large spatial extent of 5d wave functions. Using x-ray probes of magnetism and structure at high pressure, we show that compression of Sr2FeOsO6 drives an unexpected continuous change in the sign of Fe-Os exchange interactions and a transition from antiferromagnetic to ferrimagnetic order. We analyze the relevant electron-electron interactions, shedding light into fundamental differences with the more thoroughly studied 3d-3d systems.912317FAPESP - FUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULOFAPESP - FUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULO2013/14338-3Work at Argonne is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. L.S.I.V. is supported by FAPESP (SP-Brazil) under Contract No. 2013/14338-3. M.v.V. was supported by DOE-BES under Grant No. DE-FG02-03ER46097. This research was supported in part by the World Premier International Research Center of the Ministry of Education, Culture, Sports, Science and Technology (MEXT) of Japan, the Japan Society for the Promotion of Science (JSPS) through a Grant-in-Aid for Scientific Research (25289233). We would like to thank Changyong Park and Curtis Kenney-Benson for their assistance at 16-BM-D beamline, Sergey N. Tkachev for assistance with gas loading, and Richard Rosenberg for help with soft x-ray measurements. We also thank GSECARS for use of the gas loading and laser drilling facilities

Unraveling 5f-6d hybridization in uranium compounds via spin-resolved L-edge spectroscopy

FUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULO - FAPESPCOORDENAÇÃO DE APERFEIÇOAMENTO DE PESSOAL DE NÍVEL SUPERIOR - CAPESThe multifaceted character of 5f electrons in actinide materials, from localized to itinerant and in between, together with their complex interactions with 6d and other conduction electron states, has thwarted efforts for fully understanding this class of compounds. While theoretical efforts abound, direct experimental probes of relevant electronic states and their hybridization are limited. Here we exploit the presence of sizable quadrupolar and dipolar contributions in the uranium L-3-edge X-ray absorption cross section to provide unique information on the extent of spin-polarized hybridization between 5f and 6d electronic states by means of X-ray magnetic circular dichroism. As a result, we show how this 5f-6d hybridization regulates the magnetism of each sublattice in UCu2Si2 and UMn2Si2 compounds, demonstrating the potentiality of this methodology to investigate a plethora of magnetic actinide compounds.816FUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULO - FAPESPCOORDENAÇÃO DE APERFEIÇOAMENTO DE PESSOAL DE NÍVEL SUPERIOR - CAPESFUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULO - FAPESPCOORDENAÇÃO DE APERFEIÇOAMENTO DE PESSOAL DE NÍVEL SUPERIOR - CAPES10/19979-92013/22436-52014/05480-32014/26620-8Sem informaçãoWe are thankful to Roberto Caciuffo and Gerry Lander for discussions and comments on the manuscript. We thank Jose Carlos Botelho Monteiro for providing one of the UMn2Si2 samples. Work at Argonne is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC-02-06CH11357. Work at LNLS is supported by the Brazilian ministry of science and technology. This research was supported by FAPESP grants 2013/22436-5, 2014/05480-3, 10/19979-9, and 2014/26620-8. R.D.d.R. thanks the funding for his Ph.D. fellowship from CAPES brazilian agency