Electronic structure of Fe and magnetism in the 3d/5d3d/5d double perovskites Ca2_2FeReO6_6 and Ba2_2FeReO6_6

The Fe electronic structure and magnetism in (i) monoclinic Ca$_2$FeReO$_6$ with a metal-insulator transition at $T_{MI} \sim 140$ K and (ii) quasi-cubic half-metallic Ba$_2$FeReO$_6$ ceramic double perovskites are probed by soft x-ray absorption spectroscopy (XAS) and magnetic circular dichroism (XMCD). These materials show distinct Fe $L_{2,3}$ XAS and XMCD spectra, which are primarily associated with their different average Fe oxidation states (close to Fe$^{3+}$ for Ca$_2$FeReO$_6$ and intermediate between Fe$^{2+}$ and Fe$^{3+}$ for Ba$_2$FeReO$_6$) despite being related by an isoelectronic (Ca$^{2+}$/Ba$^{2+}$) substitution. For Ca$_2$FeReO$_6$, the powder-averaged Fe spin moment along the field direction ($B = 5$ T), as probed by the XMCD experiment, is strongly reduced in comparison with the spontaneous Fe moment previously obtained by neutron diffraction, consistent with a scenario where the magnetic moments are constrained to remain within an easy plane. For $B=1$ T, the unsaturated XMCD signal is reduced below $T_{MI}$ consistent with a magnetic transition to an easy-axis state that further reduces the powder-averaged magnetization in the field direction. For Ba$_2$FeReO$_6$, the field-aligned Fe spins are larger than for Ca$_2$FeReO$_6$ ($B=5$ T) and the temperature dependence of the Fe magnetic moment is consistent with the magnetic ordering transition at $T_C^{Ba} = 305$ K. Our results illustrate the dramatic influence of the specific spin-orbital configuration of Re $5d$ electrons on the Fe $3d$ local magnetism of these Fe/Re double perovskites.Comment: 7 pages, 3 figure

Investigation of element-specific and bulk magnetism, electronic and crystal structures of La{0.70}Ca{0.30}Mn{1-x}Cr{x}O{3}

The magnetic interactions in La{0.70}Ca{0.30}Mn{1-x}Cr{x}O{3} (x = 0.15, 0.50 and 0.70) are investigated by x-ray absorption spectroscopy (XAS), x-ray magnetic circular dichroism (XMCD), high-resolution x-ray powder diffraction, and bulk magnetization measurements. XAS in the Mn and Cr L{2,3} edges support stable single valent Cr{3+} ions and a varying Mn valence state with x, while the O K edge XAS spectrum reveals local maxima in the O 2p density of states close to the Fermi level due to mixing with Mn and Cr 3d states. A robust antiferromagnetic state is found for x=0.70 below TN = 258 K. For x=0.15, combined XMCD and bulk magnetization measurements indicate a fully polarized ferrimagnetic state for the Mn and Cr spins below Tc=224 K. For x=0.50, a reduced ferrimagnetic component dominated by Mn spins is present below Tc=154 K. No evidence of lattice anomalies due to cooperative charge and orbital orderings is found by x-ray diffraction for all samples. The magnetic properties of this system are rationalized in terms of a competition of ferromagnetic Mn-Mn double exchange and antiferromagnetic Cr-Cr and Cr-Mn superexchange interactions.Comment: 25 pages, 9 figure

Experimental and theoretical evidences for the ice regime in planar artificial spin ices

In this work, we explore a kind of geometrical effect in the thermodynamics of artificial spin ices (ASI). In general, such artificial materials are athermal. Here, We demonstrate that geometrically driven dynamics in ASI can open up the panorama of exploring distinct ground states and thermally magnetic monopole excitations. It is shown that a particular ASI lattice will provide a richer thermodynamics with nanomagnet spins experiencing less restriction to flip precisely in a kind of rhombic lattice. This can be observed by analysis of only three types of rectangular artificial spin ices (RASI). Denoting the horizontal and vertical lattice spacings by a and b, respectively, then, a RASI material can be described by its aspect ratio $\gamma$=a/b. The rhombic lattice emerges when $\gamma$=$\sqrt{3}$. So, by comparing the impact of thermal effects on the spin flips in these three appropriate different RASI arrays, it is possible to find a system very close to the ice regime

Exchange bias in GeMn nanocolumns: the role of surface oxidation

We report on the exchange biasing of self-assembled ferromagnetic GeMn nanocolumns by GeMn-oxide caps. The x-ray absorption spectroscopy analysis of this surface oxide shows a multiplet fine structure that is typical of the Mn2+ valence state in MnO. A magnetization hysteresis shift |HE|~100 Oe and a coercivity enhancement of about 70 Oe have been obtained upon cooling (300-5 K) in a magnetic field as low as 0.25 T. This exchange bias is attributed to the interface coupling between the ferromagnetic nanocolumns and the antiferromagnetic MnO-like caps. The effect enhancement is achieved by depositing a MnO layer on the GeMn nanocolumns.Comment: 7 pages, 5 figure

Parasitic phases at the origin of magnetic moment in BiFeO3 thin films grown by low deposition rate RF sputtering

FUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULO - FAPESPCONSELHO NACIONAL DE DESENVOLVIMENTO CIENTÍFICO E TECNOLÓGICO - CNPQA series of epitaxial BiFeO3 thin films has been grown under high partial pressure in a pure O-2 atmosphere, which leads to a low deposition rate. The samples grown under these conditions have presented an evolution of the quality of the epitaxy as the deposition temperature increases, however, spurious beta-Bi2O3 and supertetragonal BiFeO3 phases are present in the films grown at higher temperatures. The presence of gamma-Fe2O3 is reported in one growing condition, and has been attributed to the origin of hysteretic ferromagnetic behavior. A second kind of magnetism, with higher magnetic moment and anhysteretic behaviour, is attributed to the presence of mixed phases of BiFeO3.1221215FUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULO - FAPESPCONSELHO NACIONAL DE DESENVOLVIMENTO CIENTÍFICO E TECNOLÓGICO - CNPQFUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULO - FAPESPCONSELHO NACIONAL DE DESENVOLVIMENTO CIENTÍFICO E TECNOLÓGICO - CNPQ2012/18397-12012/51198-2309354/2015-3This work was supported by FAPESP (Project No. 2012/51198-2). Some of the XRD measurements were performed at the XRD2 beamline of the LNLS/CNPEM under Project Nos. 20150162 and 20160908. The authors thank the LNNano/CNPEM for XRD/XRR, AFM and sputtering facilities, the LIEC/UFSCar for the SQUID measurements, and M. M. Soares for important discussions regarding the structural characterization. P.S. thanks FAPESP for financial support (Project No. 2012/18397-1). J.C.C. acknowledges support from CNPq (Project No. 309354/2015-3)

The spin state transition in LaCoO3_{3}; revising a revision

Using soft x-ray absorption spectroscopy and magnetic circular dichroism at the Co-$L_{2,3}$ edge we reveal that the spin state transition in LaCoO$_{3}$ can be well described by a low-spin ground state and a triply-degenerate high-spin first excited state. From the temperature dependence of the spectral lineshapes we find that LaCoO$_{3}$ at finite temperatures is an inhomogeneous mixed-spin-state system. Crucial is that the magnetic circular dichroism signal in the paramagnetic state carries a large orbital momentum. This directly shows that the currently accepted low-/intermediate-spin picture is at variance. Parameters derived from these spectroscopies fully explain existing magnetic susceptibility, electron spin resonance and inelastic neutron data

Ising magnetism and ferroelectricity in Ca3_3CoMnO6_6

The origin of both the Ising chain magnetism and ferroelectricity in Ca$_3$CoMnO$_6$ is studied by $ab$ $initio$ electronic structure calculations and x-ray absorption spectroscopy. We find that Ca$_3$CoMnO$_6$ has the alternate trigonal prismatic Co$^{2+}$ and octahedral Mn$^{4+}$ sites in the spin chain. Both the Co$^{2+}$ and Mn$^{4+}$ are in the high spin state. In addition, the Co$^{2+}$ has a huge orbital moment of 1.7 $\mu_B$ which is responsible for the significant Ising magnetism. The centrosymmetric crystal structure known so far is calculated to be unstable with respect to exchange striction in the experimentally observed $\uparrow\uparrow\downarrow\downarrow$ antiferromagnetic structure for the Ising chain. The calculated inequivalence of the Co-Mn distances accounts for the ferroelectricity.Comment: 4 pages, 3 figures, PRL in press (changes made upon referees comments

Evolution of magnetic phases and orbital occupation in (SrMnO3)n/(LaMnO3)2n superlattices

The magnetic and electronic modifications induced at the interfaces in (SrMnO$_{3}$)$_{n}$/(LaMnO$_{3}$)$_{2n}$ superlattices have been investigated by linear and circular magnetic dichroism in the Mn L$_{2,3}$ x-ray absorption spectra. Together with theoretical calculations, our data demonstrate that the charge redistribution across interfaces favors in-plane ferromagnetic (FM) order and $e_{g}(x^{2}-y^{2})$ orbital occupation, in agreement with the average strain. Far from interfaces, inside LaMnO$_3$, electron localization and local strain favor antiferromagnetism (AFM) and $e_{g}(3z^{2}-r^{2})$ orbital occupation. For $n=1$ the high density of interfacial planes ultimately leads to dominant FM order forcing the residual AFM phase to be in-plane too, while for $n \geq 5$ the FM layers are separated by AFM regions having out-of-plane spin orientation.Comment: accepted for publication as a Rapid Communication in Physical Review