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Register a new userNature of the magnetism of iridium in the double perovskite Sr2CoIrO6
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We report on our investigation on the magnetism of the iridate double perovskite Sr$_2$CoIrO$_6$, a nominally Ir$^{5+}$ Van Vleck $J_{eff}=0$ system. Using x-ray absorption (XAS) and x-ray magnetic circular dichroism (XMCD) spectroscopy at the Ir-$L_{2,3}$ edges, we found a nearly zero orbital contribution to the magnetic moment and thus an apparent breakdown of the $J_{eff}=0$ ground state. By carrying out also XAS and XMCD experiments at the Co-$L_{2,3}$ edges and by performing detailed full atomic multiplet calculations to simulate all spectra, we discovered that the compound consists of about 90% Ir$^{5+}$ ($J_{eff}=0$) and Co$^{3+}$ ($S=2$) and 10% Ir$^{6+}$ ($S=3/2$) and Co$^{2+}$ ($S=3/2$). The magnetic signal of this minority Ir$^{6+}$ component is almost equally strong as that of the main Ir$^{5+}$ component. We infer that there is a competition between the Ir$^{5+}$-Co$^{3+}$ and the Ir$^{6+}$-Co$^{2+}$ configurations in this stoichiometric compound.
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We synthesize and study single crystals of a new double-perovskite Sr2YIrO6. Despite two strongly unfavorable conditions for magnetic order, namely, pentavalent Ir5+(5d4) ions which are anticipated to have Jeff=0 singlet ground states in the strong spin-orbit coupling (SOC) limit, and geometric frustration in a face centered cubic structure formed by the Ir5+ ions, we observe this iridate to undergo a novel magnetic transition at temperatures below 1.3 K. We provide compelling experimental and theoretical evidence that the origin of magnetism is in an unusual interplay between strong non-cubic crystal fields and intermediate-strength SOC. Sr2YIrO6 provides a rare example of the failed dominance of SOC in the iridates.
The synthesis and characterization of the previously unknown material LaCaScIrO$_6$ is reported. LaCaScIrO$_6$ presents a new example of the rare case of a double perovskite with the strongly spin-orbit coupled 5textit{d}-ion Ir$^{4+}$ as its only magnetic species, forming a monoclinically distorted version of the frustrated fcc lattice. Magnetization measurements show a weak anomaly at 8~K. The Curie-Weiss temperature Theta$_{CW}$ and effective magnetic moment mu$_{eff}$ of LaCaScIrO$_6$ are in close proximity to the related compound La$_2$MgIrO$_6$ but differ from La$_2$ZnIrO$_6$. This suggests that the nature of the non-magnetic textit{B}-ion, namely its textit{d}-orbital filling has a strong influence on the magnetic properties. The textit{d}$^{0}$-ions Sc$^{3+}$ and Mg$^{2+}$ allow a different kind of exchange interactions within the Ir-sublattice than the textit{d}$^{10}$-ion Zn$^{2+}$. In addition, ac-susceptibility data does not show signs of a spin-glass ground state. The nature of the magnetism in LaCaScIrO$_6$ has been further elucidated using muon spin relaxation measurements. The zero-field measurements reveal the absence of well defined oscillations down to 1.6,K, while temperature dependent $mu$SR studies show an anomaly at 8,K. Overall, our results suggest the presence of two different magnetic environments or domains in LaCaScIrO$_6$, which is likely related to its structural features.
We present detailed calculations of the electric field gradient (EFG) using a point charge approximation in Ba$_2$NaOsO$_6$, a Mott insulator with strong spin-orbit interaction. Recent $^{23}$Na nuclear magnetic resonance (NMR) measurements found that the onset of local point symmetry breaking, likely caused by the formation of quadrupolar order, precedes the formation of long range magnetic order in this compound. An extension of the static $^{23}$Na NMR measurements as a function of the orientation of a 15 T applied magnetic field at 8 K in the magnetically ordered phase is reported. Broken local cubic symmetry induces a non-spherical electronic charge distribution around the Na site and thus finite EFG, affecting the NMR spectral shape. We combine the spectral analysis as a function of the orientation of the magnetic field with calculations of the EFG to determine the exact microscopic nature of the lattice distortions present in low temperature phases of this material. We establish that orthorhombic distortions, constrained along the cubic axes of the perovskite reference unit cell, of oxygen octahedra surrounding Na nuclei are present in the magnetic phase. Other common types of distortions often observed in oxide structures are considered as well.
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.
The temperature dependence of the manganese magnetic moment and the spin-lattice relaxation rate measured by the muon spin relaxation technique in the magnetically ordered phase of the chiral intermetallic cubic MnSi system are both explained in terms of helimagnon excitations of a localized spin model. The two free parameters characterizing the helimagnon dispersion relation are determined. A combined analysis of the two data sets cannot be achieved using the self-consistent renormalization theory of spin fluctuations which assumes the magnetism of MnSi to arise uniquely from electronic bands. As a result of this work, MnSi is proposed to be a dual electronic system composed of localized and itinerant magnetic electrons. Finally we note that the analysis framework can be applied to other helimagnets such as the magnetoelectric compound Cu2OSeO3.
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