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Hyperfine interaction and electronic spin fluctuation study on Sr$_{2-x}$La$_x$FeCoO$_6$ (x = 0, 1, 2) by high-resolution back-scattering neutron spectroscopy

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 Added by Tapan Chatterji
 Publication date 2018
  fields Physics
and research's language is English




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The study of hyperfine interaction by high-resolution inelastic neutron scattering is not very well known compared to the other competing techniques viz. NMR, Mossbauer, PACS etc. Also the study is limited mostly to magnetically ordered systems. Here we report such study on Sr$_{2-x}$La$_x$FeCoO$_6$ (x = 0, 1, 2) of which first (Sr$_2$FeCoO$_6$ with x = 0) has a canonical spin spin glass, the second (SrLaFeCoO$_6$ with x = 1) has a so-called magnetic glass and the third (La$_2$FeCoO$_6$ with x = 2) has a magnetically ordered ground state. Our present study revealed clear inelastic signal for SrLaFeCoO$_6$, possibly also inelastic signal for Sr$_2$FeCoO$_6$ below the spin freezing temperatures $T_{sf}$ but no inelastic signal at all for for the magnetically ordered La$_2$FeCoO$_6$ in the neutron scattering spectra. The broadened inelastic signals observed suggest hyperfine field distribution in the two disordered magnetic glassy systems and no signal for the third compound suggests no or very small hyperfine field at the Co nucleus due to Co electronic moment. For the two magnetic glassy system apart from the hyperfine signal due only to Co, we also observed electronic spin fluctuations probably from both Fe and Co electronic moments. end{abstract}



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The magnetism of the double perovskite compounds SLFCOx ($x$ = 0, 1, 2) are contrasted using magnetization, neutron diffraction and electron paramagnetic resonance with the support from density functional theory calculations. LFCO is identified as a long-range ordered antiferromagnet displaying a near-room temperature transition at $T_N$ = 270~K, accompanied by a low temperature structural phase transition at $T_S$ = 200~K. The structural phase transformation at $T_S$ occurs from $Roverline{3}c$ at 300~K to $Pnma$ at 200~K. The density functional theory calculations support an insulating non-compensated AFM structure. The long-range ordered magnetism of LFCO transforms to short-range glassy magnetism as La is replaced with Sr in the other two compounds. The magnetism of LFCO is differentiated from the non-equilibrium glassy features of SFCO and SLFCO using the {em cooling-and-heating-in-unequal-fields} (CHUF) magnetization protocols. This contransting magnetism in the SLFCOx series is evidenced in electron paramegnetic resonance studies. The electronic density-of-states estimated using the density functional theory calculations contrast the insulating feature of LFCO from the metallic nature of SFCO. From the present suite of experimental and computational results on SLFCOx, it emerges that the electronic degrees of freedom, along with antisite disorder, play an important role in controlling the magnetism observed in double perovskites.
We have investigated the electronic structure of electron-doped Sr$_{2-x}$La$_x$FeMoO$_6$ ($x$=0.0 and 0.2) by photoemission spectroscopy and band-structure calculations within the local-density approximation+$U$ (LDA+$U$) scheme. A characteristic double-peak feature near the Fermi level ($E_{rm F}$) has been observed in the valence-band photoemission spectra of both $x$=0.0 and 0.2 samples. A photon-energy dependence of the spectra in the Mo 4$d$ Cooper minimum region compared with the band-structure calculations has shown that the first peak crossing $E_{rm F}$ consists of the (Fe+Mo) $t_{2gdownarrow}$ states (feature A) and the second peak well below $E_{rm F}$ is dominated by the Fe $e_{guparrow}$ states (feature B). Upon La substitution, the feature A moves away from $E_{rm F}$ by $sim$50 meV which is smaller than the prediction of our band theory, 112 meV. In addition, an intensity enhancement of $both$ A and B has been observed, although B is not crossing $E_{rm F}$. Those two facts are apparently incompatible with the simple rigid-band shift due to electron doping. We point out that such phenomena can be understood in terms of the strong Hunds rule energy stabilization in the 3$d^5$ configuration at the Fe sites in this compound. From an observed band-narrowing, we have also deduced a mass enhancement of $sim$2.5 with respect to the band theory, in good agreement with a specific heat measurement.
We have studied Ir spin and orbital magnetic moments in the double perovskites La$_{2-x}$Sr$_x$CoIrO$_6$ by x-ray magnetic circular dichroism. In La$_2$CoIrO$_6$, Ir$^{4+}$ couples antiferromagnetically to the weak ferromagnetic moment of the canted Co$^{2+}$ sublattice and shows an unusually large negative total magnetic moment (-0.38,$mu_{text B}$/f.u.) combined with strong spin-orbit interaction. In contrast, in Sr$_2$CoIrO$_6$, Ir$^{5+}$ has a paramagnetic moment with almost no orbital contribution. A simple kinetic-energy-driven mechanism including spin-orbit coupling explains why Ir is susceptible to the induction of substantial magnetic moments in the double perovskite structure.
We have investigated the ferromagnetic phase transition of elemental Co by high-resolution neutron backscattering spectroscopy. We monitored the splitting of the nuclear levels by the hyperfine field at the Co nucleus. The energy of this hyperfine splitting is identified as the order parameter of the ferromagnetic phase transition. By measuring the temperature dependence of the energy we determined the critical exponent $beta = 0.350 pm 0.002$ and the ferromagnetic Curie temperature of $T_{text{C}} = 1400$~K. The present result of the critical exponent agrees better with the predicted value (0.367) of the 3-dimensional Heisenberg model than that determined previously by NMR.
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We report the first empirical demonstration that resonant inelastic x-ray scattering (RIXS) is sensitive to emph{collective} magnetic excitations in $S=1$ systems by probing the Ni $L_3$-edge of La$_{2-x}$Sr$_x$NiO$_4$ ($x = 0, 0.33, 0.45$). The magnetic excitation peak is asymmetric, indicating the presence of single and multi spin-flip excitations. As the hole doping level is increased, the zone boundary magnon energy is suppressed at a much larger rate than that in hole doped cuprates. Based on the analysis of the orbital and charge excitations observed by RIXS, we argue that this difference is related to the orbital character of the doped holes in these two families. This work establishes RIXS as a probe of fundamental magnetic interactions in nickelates opening the way towards studies of heterostructures and ultra-fast pump-probe experiments.
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