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Register a new userRevisiting Goodenough-Kanamori rules in a new series of double perovskites LaSr$_{1-x}$Ca$_x$NiReO$_6$
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The magnetic ground state in highly ordered double perovskites LaSr$_{1-x}$Ca$_x$NiReO$_6$ ($x$ = 0.0, 0.5, 1.0) were studied in view of the Goodenough-Kanamori rules of superexchange interactions. In LaSrNiReO$_6$, Ni and Re sublattices are found to exhibit curious magnetic states, but do not show any long range magnetic ordering. The magnetic transition at $sim$ 255 K is identified with the Re sublattic magnetic ordering. The sublattice interactions are tuned by modifying the Ni-O-Re bond angles via changing the lattice structure through Ca doping. Upon Ca doping, the Ni and Re sublattices start to display a ferrimagnetically ordered state at low temperature. The neutron powder diffraction reveals a canted alignment between the Ni and the Re sublattices, while the individual sublattice is ferromagnetic. The transition temperature of the ferrimagnetic phase increases monotonically with increasing Ca concentration.
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Spin-orbit coupling (SOC) plays a crucial role in magnetic and electronic properties of 5$d$ iridates. In this paper we have experimentally investigated the structural and physical properties of a series of Ir-based double perovskite compounds Pr$_{2-x}$Sr$_x$MgIrO$_6$ ($x$ = 0, 0.5, 1; hereafter abbreviated as PMIO, PSMIO1505, and PSMIO). Interestingly, these compounds have recently been proposed to undergo a transition from the spin-orbit-coupled Mott insulating phase at $x$ = 0 to the elusive half-metallic antiferromagnetic (HMAFM) state with Sr doping at $x$ = 1. However, our detailed magnetic and electrical measurements refute any kind of HMAFM possibility in either of the doped samples. In addition, we establish that within these Pr$_{2-x}$Sr$_x$MgIrO$_6$ double perovskites, changes in Ir-oxidation states (4+ for PMIO to 5+ for PSMIO via mixed 4+/5+ for PSMIO1505) lead to markedly different magnetic behaviors. While SOC on Ir is at the root of the observed insulating behaviors for all three samples, the correlated magnetic properties of these three compounds develop entirely due to the contribution from local Ir moments. Additionally, the magnetic Pr$^{3+}$ (4$f^2$) ions, instead of showing any kind of ordering, only contribute to the total paramagnetic moment. It is seen that the PrSrMgIrO$_6$ sample does not order down to 2 K despite antiferromagnetic interactions. But, the $d^5$ iridate Pr$_2$MgIrO$_6$ shows a sharp antiferromagnetic (AFM) transition at around 14 K, and in the mixed valent Pr$_{1.5}$Sr$_{0.5}$MgIrO$_6$ sample the AFM transition is shifted to a much lower temperature ($sim$ 6 K) due to weakening of the AFM exchange.
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 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.
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.
We investigate the doping-induced changes in the electronic structure of CeB$_6$ on a series of substituted Ce$_{1-x}R_x$B$_6$ samples ($R$ = La, Nd) using diffuse neutron scattering. We observe a redistribution of magnetic spectral weight across the Brillouin zone, which we associate with the changes in the Fermi-surface nesting properties related to the modified charge carrier concentration. In particular, a strong diffuse peak at the corner of the Brillouin zone ($R$ point), which coincides with the propagation vector of the elusive antiferroquadrupolar (AFQ) order in CeB$_6$, is rapidly suppressed by both La and Nd doping, like the AFQ order itself. The corresponding spectral weight is transferred to the $X(00frac{1}{2})$ point, ultimately stabilizing a long-range AFM order at this wave vector at the Nd-rich side of the phase diagram. At an intermediate Nd concentration, a broad diffuse peak with multiple local maxima of intensity is observed around the $X$ point, evidencing itinerant frustration that gives rise to multiple ordered phases for which Ce$_{1-x}$Nd$_x$B$_6$ is known. On the La-rich side of the phase diagram, however, dilution of the magnetic moments prevents the formation of a similar $(00frac{1}{2})$-type order despite the presence of nesting. Our results demonstrate how diffuse neutron scattering can be used to probe the nesting vectors in complex f-electron systems directly, without reference to the single-particle band structure, and emphasize the role of Fermi surface geometry in stabilizing magnetic order in rare-earth hexaborides.
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