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Register a new userA variety of elastic anomalies in orbital-active nearly-itinerant cobalt vanadate spinel
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We perform ultrasound velocity measurements on a single crystal of nearly-metallic spinel Co$_{1.21}$V$_{1.79}$O$_4$ which exhibits a ferrimagnetic phase transition at $T_C sim$ 165 K. The experiments reveal a variety of elastic anomalies in not only the paramagnetic phase above $T_C$ but also the ferrimagnetic phase below $T_C$, which should be driven by the nearly-itinerant character of the orbitally-degenerate V 3$d$ electrons. In the paramagnetic phase above $T_C$, the elastic moduli exhibit elastic-mode-dependent unusual temperature variations, suggesting the existence of a dynamic spin-cluster state. Furthermore, above $T_C$, the sensitive magnetic-field response of the elastic moduli suggests that, with the negative magnetoresistance, the magnetic-field-enhanced nearly-itinerant character of the V 3$d$ electrons emerges from the spin-cluster state. This should be triggered by the inter-V-site interactions acting on the orbitally-degenerate 3$d$ electrons. In the ferrimagnetic phase below $T_C$, the elastic moduli exhibit distinct anomalies at $T_1sim$ 95 K and $T_2sim$ 50 K, with a sign change of the magnetoresistance at $T_1$ (positive below $T_1$) and an enhancement of the positive magnetoresistance below $T_2$, respectively. These observations below $T_C$ suggest the successive occurrence of an orbital glassy order at $T_1$ and a structural phase transition at $T_2$, where the rather localized character of the V 3$d$ electrons evolves below $T_1$ and is further enhanced below $T_2$.
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We have investigated the orbital states of the orbital-glassy (short-range orbital ordered) spinel vanadate Co$_{1.21}$V$_{1.79}$O$_{4}$ using x-ray absorption spectroscopy (XAS), x-ray magnetic circular dichroism (XMCD), and subsequent configuration-interaction cluster-model calculation. From the sign of the XMCD spectra, it was found that the spin magnetic moment of the Co ion is aligned parallel to the applied magnetic field and that of the V ion anti-parallel to it, consistent with neutron scattering studies. It was revealed that the excess Co ions at the octahedral site take the trivalent low-spin state, and induce a random potential to the V sublattice. The orbital magnetic moment of the V ion is small although finite, suggesting that the ordered orbitals mainly consists of real-number orbitals.
The crossover from localized- to itinerant-electron behavior is associated with many intriguing phenomena in condensed-matter physics. In this paper, we investigate the crossover from localized to itinerant regimes in the spinel system Mn$_{1-x}$Co$_x$V$_2$O$_4$. At low Co doping, orbital order (OO) of the localized electrons on the V3+ ions suppresses magnetic frustration by triggering a tetragonal distortion. With Co doping, electronic itinerancy melts the OO and suppresses the structural phase transition while the reduced spin-lattice coupling produces magnetic frustration. Neutron scattering measurements and first-principles-guided spin models reveal that the non-collinear state at high Co doping is produced by weakened local anisotropy and enhanced Co-V spin interactions.
The realization of Kitaevs honeycomb magnetic model in real materials has become one of the most pursued topics in condensed matter physics and materials science. If found, it is expected to host exotic quantum phases of matter and offers potential realizations of fault$-$tolerant quantum computations. Over the past years, much effort was made on 4d$-$ or 5d$-$ heavy transition metal compounds because of their intrinsic strong spin$-$orbit coupling. But more recently, there have been growing shreds of evidence that the Kitaev model could also be realized in 3d$-$transition metal systems with much weaker spin$-$orbit coupling. This review intends to serve as a guide to this fast$-$developing field focusing on systems with d$^7$ transition metal occupation. It overviews the current theoretical and experimental progress on realizing the Kitaev model in those systems. We examine the recent experimental observations of candidate materials with Co$^{2+}$ ions: e.g., CoPS$_3$, Na$_3$Co$_2$SbO$_6$, and Na$_2$Co$_2$TeO$_6$, followed by a brief review of theoretical backgrounds. We conclude this article by comparing experimental observations with density functional theory (DFT) calculations. We stress the importance of inter$-t_{2g}$ hopping channels and Hunds coupling in the realization of Kitaev interactions in Co$-$based compounds, which has been overlooked in previous studies. This review suggests future directions in the search for Kitaev physics in 3d cobalt compounds and beyond.
The chemical pressure effect on the structural, transport, magnetic and electronic properties (by measuring X-ray photoemission spectroscopy) of ZnV2O4 has been investigated by doping Mn and Co on the Zinc site of ZnV2O4. With Mn doping the V-V distance increases and with Co doping it decreases. The resistivity and thermoelectric power data indicate that as the V-V distance decreases the system moves towards Quantum Phase Transition. The transport data also indicate that the conduction is due to the small polaron hopping. The chemical pressure shows the non-monotonous behaviour of charge gap and activation energy. The XPS study also supports the observation that with decrease of the V-V separation the system moves towards Quantum Phase Transition. On the other hand when Ti is doped on the V-site of ZnV2O4 the metal-metal distance decreases and at the same time the TN also increases.
We use x-ray spectroscopy at Ir L$_3$/L$_2$ absorption edge to study powder samples of the intercalated honeycomb magnet Ag$_3$LiIr$_2$O$_6$. Based on x-ray absorption and resonant inelastic x-ray scattering measurements, and exact diagonalization calculations including next-neighbour Ir-Ir electron hoping integrals, we argue that the intercalation of Ag atoms results in a nearly itinerant electronic structure with enhanced Ir-O hybridization. As a result of the departure from the local relativistic $j_{rm eff}! = !1/2$ state, we find that the relative orbital contribution to the magnetic moment is increased, and the magnetization density is spatially extended and asymmetric. Our results confirm the importance of metal - ligand hybridazation in the magnetism of transition metal oxides and provide empirical guidance for understanding the collective magnetism in intercalated honeycomb iridates.
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