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Register a new userLocal magnetism and spin correlations in the geometrically frustrated cluster magnet LiZn$_2$Mo$_3$O$_8$
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LiZn$_2$Mo$_3$O$_8$ has been proposed to contain $S~=~1/2$ Mo$_3$O$_{13}$ magnetic clusters arranged on a triangular lattice with antiferromagnetic nearest-neighbor interactions. Here, microwave and terahertz electron spin resonance (ESR), $^7$Li nuclear magnetic resonance (NMR), and muon spin rotation ($mu textrm{SR}$) spectroscopies are used to characterize the local magnetic properties of LiZn$_2$Mo$_3$O$_8$. These results show the magnetism in LiZn$_2$Mo$_3$O$_8$ arises from a single isotropic $S~=~1/2$ electron per cluster and that there is no static long-range magnetic ordering down to $T~=~0.07,textrm{K}$. Further, there is evidence of gapless spin excitations with spin fluctuations slowing down as the temperature is lowered. These data indicate strong spin correlations which, together with previous data, suggest a low-temperature resonating valence-bond state in LiZn$_2$Mo$_3$O$_8$.
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LiZn$_2$Mo$_3$O$_8$ is an electrically insulating geometrically frustrated antiferromagnet in which inorganic Mo$_3$O$_{13}$ clusters each behaves as a single $S = 1/2$ unit, with the clusters arranged on a two-dimensional triangular lattice. Prior results have shown that LiZn$_2$Mo$_3$O$_8$ does not exhibit static magnetic order down to at least $T = 0.05,K$, and instead possesses a valence bond ground state. Here, we show that LiZn$_2$Mo$_3$O$_8$ can be hole doped by oxidation with $mathrm{I}_2$ and subsequent removal of $mathrm{Zn}^{2+}$ cations to access the entire range of electron count, from one to zero unpaired electrons per site on the triangular lattice. Contrary to expectations, no metallic state is induced; instead, the primary effect is to suppress the number of sites contributing to the condensed valence-bond state. Further, diffraction and pair-distribution function analysis show no evidence for local Jahn-Teller distortions or other deviations from the parent trigonal symmetry as a function of doping or temperature. Taken together, the data and density functional theory calculations indicate that removal of electrons from the magnetic layers favors Anderson localization of the resulting hole and an increase in the electrical band-gap over the formation of a metallic and superconducting state. These results put strong constraints on the chemical conditions necessary to realize metallic states from parent insulating geometrically frustrated antiferromagnets.
We have measured the thermal conductivity of the geometrically frustrated quasi-onedimensional spin system Cu$_3$Mo$_2$O$_9$ in magnetic fields. A contribution of the thermal conductivity due to spins has been observed in the thermal conductivity along the spin chains. The thermal conductivity due to phonons, $kappa_{rm phonon}$, has been found to decrease by the application of a magnetic field, which has been explained as being due to the reduction in the spin gap originating from the spin-singlet dimers. Moreover, it has been found that $kappa_{rm phonon}$ increases with increasing field in high fields above ~7 T at low temperatures. This suggests the existence of a novel field-induced spin state and is discussed in terms of the possible spin-chirality ordering in a frustrated Mott insulator.
We report single-crystal neutron diffraction studies on a spinel antiferromagnet GeCo$_2$O$_4$, which exhibits magnetic order with a trigonal propagation vector and tetragonal lattice expansion ($c/asimeq1.001$) below $T_{rm N}=21$ K. For this inconsistency between spin and lattice in symmetry, magnetic Bragg reflections with a tetragonal propagation vector were discovered below $T_{rm N}$. We discuss spin and orbital states of Co$^{2+}$ ion underlying the new magnetic component.
We report on the structural and spectroscopic characterization of the multiferroic Fe$_2$Mo$_3$O$_8$. Synchrotron x-ray and neutron diffraction, as well as thermal expansion measurements reveal a lattice anomaly at $T_{mathrm{N}}simeq 60,$K but do not show any symmetry lowering in the magnetically ordered state. The lattice parameter $c$ exhibits a non-monotonic behavior with a pronounced minimum around $200,$K, which is also reflected in an anomalous behavior of some of the observed infrared-active optical excitations and parallels the onset of short-range magnetic order. The infrared reflectivity spectra measured between 5 and 300$,$K in the frequency range of $100-8000,$cm$^{-1}$ reveal most of the expected phonon modes in comparison with the eigenfrequencies obtained by density-functional calculations. The $A_1$ phonons show an overall hardening upon cooling, whereas a non-monotonic behavior is observed for some of the $E_1$ modes. These modes also show a strongly increased phonon lifetime below $T_mathrm{N}$, which we associate with the quenched direction of the orbital moment in the magnetically ordered state. A similar increase is observed in the lifetime of the higher-lying $d$-$d$ excitations of the tetrahedral Fe$^{2+}$ site, which become clearly visible below $T_mathrm{N}$ only.
We report neutron scattering studies of the spin correlations of the geometrically frustrated pyrochlore Tb2Mo2O7 using single crystal samples. This material undergoes a spin-freezing transition below Tg~24 K, similar to Y2Mo2O7, and has little apparent chemical disorder. Diffuse elastic peaks are observed at low temperatures, indicating short-range ordering of the Tb moments in an arrangement where the Tb moments are slightly rotated from the preferred directions of the spin ice structure. In addition, a Q-independent signal is observed which likely originates from frozen, but completely uncorrelated, Tb moments. Inelastic measurements show the absence of sharp peaks due to crystal field excitations. These data show how the physics of the Tb sublattice responds to the glassy behavior of the Mo sublattice with the associated effects of lattice disorder.
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