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Register a new userObservation of elastic anomalies driven by coexisting dynamical spin Jahn-Teller effect and dynamical molecular spin state in paramagnetic phase of the frustrated MgCr$_2$O$_4$$
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Ultrasound velocity measurements of magnesium chromite spinel MgCr$_2$O$_4$ reveal elastic anomalies in the paramagnetic phase that are characterized as due to geometrical frustration. The temperature dependence of the tetragonal shear modulus $(C_{11}-C_{12})/2$ exhibits huge Curie-type softening, which should be the precursor to spin Jahn-Teller distortion in the antiferromagnetic phase. The trigonal shear modulus $C_{44}$ exhibits nonmonotonic temperature dependence with a characteristic minimum at $sim$50 K, indicating a coupling of the lattice to dynamical molecular spin state. These results strongly suggest the coexistence of dynamical spin Jahn-Teller effect and dynamical molecular spin state in the paramagnetic phase, which is compatible with the coexistence of magnetostructural order and dynamical molecular spin state in the antiferromagnetic phase.
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Ultrasound velocity measurements were performed on a single crystal of spin-frustrated ferrite spinel ZnFe$_2$O$_4$ from 300 K down to 2 K. In this cubic crystal, all the symmetrically-independent elastic moduli exhibit softening with a characteristic minimum with decreasing temperature below $sim$100 K. This elastic anomaly suggests a coupling between dynamical lattice deformations and molecular-spin excitations. In contrast, the elastic anomalies, normally driven by the magnetostructural phase transition and its precursor, are absent in ZnFe$_2$O$_4$, suggesting that the spin-lattice coupling cannot play a role in relieving frustration within this compound. The present study infers that, for ZnFe$_2$O$_4$, the dynamical molecular-spin state evolves at low temperatures without undergoing precursor spin-lattice fluctuations and spin-lattice ordering. It is expected that ZnFe$_2$O$_4$ provides the unique dynamical spin-lattice liquid-like system, where not only the spin molecules but also the cubic lattice fluctuate spatially and temporally.
Ultrasound velocity measurements of cubic spinel GeCo$_2$O$_4$ in single crystal were performed for the investigation of shear and compression moduli. The shear moduli in the paramagnetic state reveal an absence of Jahn-Teller activity despite the presence of orbital degeneracy in the Co$^{2+}$ ions. Such a Jahn-Teller inactivity indicates that the intersite orbital-orbital interaction is much stronger than the Jahn-Teller coupling. The compression moduli in the paramagnetic state near the N$acute{e}$el temperature $T_N$ reveal that the most relevant exchange path for the antiferromagnetic transition lies in the [111] direction. This exchange-path anisotropy is consistent with the antiferromagnetic structure with the wave vector $q parallel$ [111], suggesting the presence of bond frustration due to competition among a direct ferromagnetic and several distant-neighbors antiferromagnetic interactions. In the JT-inactive condition, the bond frustration can be induced by geometrical orbital frustration of $t_{2g}$-$t_{2g}$ interaction between the Co$^{2+}$ ions which can be realized in the pyrochlore lattice of the high spin Co$^{2+}$ with $t_{2g}$-orbital degeneracy. In GeCo$_2$O$_4$, the tetragonal elongation below $T_N$ releases the orbital frustration by quenching the orbital degeneracy.
Ultrasound velocity measurements of the orbitally-frustrated GeCo$_2$O$_4$ reveal unusual elastic instabilities due to the phonon-spin coupling within the antiferromagnetic phase. Shear moduli exhibit anomalies arising from the coupling to short-range ferromagnetic excitations. Diplike anomalies in the magnetic-field dependence of elastic moduli reveal magnetic-field-induced orbital order-order transitions. These results strongly suggest the presence of geometrical orbital frustration which causes novel orbital phenomena within the antiferromagnetic phase.
The low-dimensional s=1/2 compound (NO)[Cu(NO3)3] has recently been suggested to follow the Nersesyan-Tsvelik model of coupled spin chains. Such a system shows unbound spinon excitations and a resonating valence bond ground state due spin frustration. Our Raman scattering study demonstrates phonon anomalies as well as the suppression of a broad magnetic scattering continuum for temperatures below a characteristic temperature, T<T*=100K. We interpret these effects as evidence for a dynamical interplay of spin and lattice degrees of freedom that might lead to a further transition into a dimerized or structurally distorted phase at lower temperatures.
We consider the superexchange in `frustrated Jahn-Teller systems, such as the transition metal oxides NaNiO_2, LiNiO_2, and ZnMn_2O_4, in which transition metal ions with doubly degenerate orbitals form a triangular or pyrochlore lattice and are connected by the 90-degree metal-oxygen-metal bonds. We show that this interaction is much different from a more familiar exchange in systems with the 180-degree bonds, e.g. perovskites. In contrast to the strong interplay between the orbital and spin degrees of freedom in perovskites, in the 90-degree exchange systems spins and orbitals are decoupled: the spin exchange is much weaker than the orbital one and it is ferromagnetic for all orbital states. Due to frustration, the mean-field orbital ground state is strongly degenerate. Quantum orbital fluctuations select particular ferro-orbital states, such as the one observed in NaNiO_2. We also discuss why LiNiO_2 may still behave as an orbital liquid.
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