No Arabic abstract
In order to assess the magnetic ordering process in Fe2VAl and the related material Fe2VGa, we have carried out nuclear magnetic resonance (NMR) and Mossbauer studies. 27Al NMR relaxation measurements covered the temperature range 4 -- 500 K in Fe(2+x)V(1-x)Al samples. We found a peak in the NMR spin-lattice relaxation rate, 27T1^-1, corresponding to the magnetic transitions in each of these samples. These peaks appear at 125 K, 17 K, and 165 K for x = 0.10, 0, and - 0.05 respectively, and we connect these features with critical slowing down of the localized antisite defects. Mossbauer measurements for Fe2VAl and Fe2VGa showed lines with no hyperfine splitting, and isomer shifts nearly identical to those of the corresponding sites in Fe3Al and Fe3Ga, respectively. We show that a model in which local band filling leads to magnetic regions in the samples, in addition to the localized antisite defects, can account for the observed magnetic ordering behavior.
We used angle-resolved photoemission spectroscopy (ARPES) and density functional theory calculations to study the electronic structure of Ba(Fe1-x-yCoxMny)2As2 for x=0.06 and 0<=y <=0.07. From ARPES we derive that the substitution of Fe by Mn does not lead to hole doping, indicating a localization of the induced holes. An evaluation of the measured spectral function does not indicate a diverging effective mass or scattering rate near optimal doping. Thus the present ARPES results indicate a continuous evolution of the quasiparticle interaction and therefore question previous quantum critical scenarios.
The electronic structure of the magnetic semiconductor Ga$_{1-x}$Cr$_{x}$N and the effect of Si doping on it have been investigated by photoemission and soft x-ray absorption spectroscopy. We have confirmed that Cr in GaN is predominantly trivalent substituting for Ga, and that Cr 3$d$ states appear within the band gap of GaN just above the N 2$p$-derived valence-band maximum. As a result of Si doping, downward shifts of the core levels (except for Cr 2$p$) and the formation of new states near the Fermi level were observed, which we attribute to the upward chemical potential shift and the formation of a small amount of Cr$^{2+}$ species caused by the electron doping. Possibility of Cr-rich cluster growth by Si doping are discussed based on the spectroscopic and magnetization data.
Polarization-dependent x-ray absorption spectroscopy at the B 1s edge of single-crystalline Mg(x)Al(1-x)B(2) reveals a strongly anisotropic electronic structure near the Fermi energy. Comparing spectra for superconducting compounds (x=0.9, 1.0) with those for the non-superconductor x=0.0 gives direct evidence on the importance of an in-plane spectral feature crossing E_F for the superconducting properties of the diborides. Good agreement is found with the projected B 2p density of states from LDA band structure calculations.
The valence and spin state evolution of Mn and Co on TbMn$_{rm 1-x}$Co$_{rm x}$O$_3$ series is precisely determined by means of soft and hard x-ray absorption spectroscopy (XAS) and K$beta$ x-ray emission spectroscopy (XES). Our results show the change from Mn$^{3+}$ to Mn$^{4+}$ both high-spin (HS) together with the evolution from Co$^{2+}$ HS to Co$^{3+}$ low-spin (LS) with increasing $rm x$. In addition, high energy resolution XAS spectra on the K pre-edge region are interpreted in terms of the strong charge transfer and hybridization effects along the series. These results correlate well with the spin values of Mn and Co atoms obtained from the K$beta$ XES data. From this study, we determine that Co enters into the transition metal sublattice of TbMnO$_3$ as a divalent ion in HS state, destabilizing the Mn long range magnetic order since very low doping compositions (${rm x} le 0.1$). Samples in the intermediate composition range ($0.4 le {rm x} le 0.6$) adopt the crystal structure of a double perovskite with long range ferromagnetic ordering which is due to Mn$^{4+}$-O-Co$^{2+}$ superexchange interactions with both cations in HS configuration. Ferromagnetism vanishes for ${rm x} ge 0.7$ due to the structural disorder that collapses the double perovskite structure. The spectroscopic techniques reveal the occurrence of Mn$^{4+}$ HS and a fluctuating valence state Co$^{2+}$ HS/Co$^{3+}$ LS in this composition range. Disorder and competitive interactions lead to a magnetic glassy behaviour in these samples.
Fe$M_2X_4$ spinels, where $M$ is a transition metal and $X$ is oxygen or sulfur, are candidate materials for spin filters, one of the key devices in spintronics. We present here a computational study of the inversion thermodynamics and the electronic structure of these (thio)spinels for $M=$ Cr, Mn, Co, Ni, using calculations based on the density functional theory with on-site Hubbard corrections (DFT+$U$). The analysis of the configurational free energies shows that different behaviour is expected for the equilibrium cation distributions in these structures: FeCr$_2X_4$ and FeMn$_2$S$_4$ are fully normal, FeNi$_2X_4$ and FeCo$_2$S$_4$ are intermediate, and FeCo$_2$O$_4$ and FeMn$_2$O$_4$ are fully inverted. We have analyzed the role played by the size of the ions and by the crystal field stabilization effects in determining the equilibrium inversion degree. We also discuss how the electronic and magnetic structure of these spinels is modified by the degree of inversion, assuming that this could be varied from the equilibrium value. We have obtained electronic densities of states for the completely normal and completely inverse cation distribution of each compound. FeCr$_2X_4$, FeMn$_2X_4$, FeCo$_2$O$_4$ and FeNi$_2$O$_4$ are half-metals in the ferrimagnetic state when Fe is in tetrahedral positions. When $M$ is filling the tetrahedral positions, the Cr-containing compounds and FeMn$_2$O$_4$ are half-metallic systems, while the Co and Ni spinels are insulators. The Co and Ni sulfide counterparts are metallic for any inversion degree together with the inverse FeMn$_2$S$_4$. Our calculations suggest that the spin filtering properties of the Fe$M_2X_4$ (thio)spinels could be modified via the control of the cation distribution through variations in the synthesis conditions.