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Magnetic State of the Geometrically Frustrated Quasi-One-Dimensional Spin System Cu$_3$Mo$_2$O$_9$ Studied by Thermal Conductivity

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 Added by Takayuki Kawamata
 Publication date 2015
  fields Physics
and research's language is English




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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.



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We have measured the thermal conductivity along the [101] direction, kappa_[101]_, along the [10-1] direction, kappa_[10-1]_, and along the b-axis, kappa_b_, of the quasi one-dimensional S=1/2 spin system Sr_2_V_3_O_9_ in magnetic fields up to 14 T, in order to find the thermal conductivity due to spinons and to clarify whether the spin-chains run along the [101] or [10-1] direction. It has been found that both kappa_[101]_, kappa_[10-1]_ and kappa_b_ show one peak around 10 K in zero field and that the magnitude of kappa_[10-1]_ is larger than those of kappa_[101]_ and kappa_b_. By the application of magnetic field along the heat current, the peak of kappa_[10-1]_ is markedly suppressed, while the peaks of kappa_[101]_ and kappa_b_ little change. These results indicate that there is a large contribution of spinons to kappa_[10-1]_ and suggest that the spin-chains run along the [10-1] direction.
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$_8$.
The quantum spin liquid (QSL) is an exotic phase of magnetic materials where the spins continue to fluctuate without any symmetry breaking down to zero temperature. Among the handful reports of QSL with spin $Sge$1, examples with magnetic ions on a three-dimensional magnetic lattice are extremely rare since both larger spin and higher dimension tend to suppress quantum fluctuations. In this work, we offer a new strategy to achieve 3-D QSL with high spin by utilizing two types of transition metal ions, both are magnetically active but located at crystallographically inequivalent positions. We design a 3-D magnetic system Ba$_3$NiIr$_2$O$_9$ consisting of interconnected corner shared NiO$_6$ octahedra and face shared Ir$_2$O$_9$ dimer, both having triangular arrangements in textit{a-b} plane. X-ray absorption spectroscopy measurements confirm the presence of Ni$^{2+}$ ($S$=1). Our detailed thermodynamic and magnetic measurements reveal that this compound is a realization of gapless QSL state down to at least 100 mK. Ab-initio calculations find a strong magnetic exchange between Ir and Ni sublattices and in-plane antiferromagnetic coupling between the dimers, resulting in dynamically fluctuating magnetic moments on both the Ir and Ni sublattice.
Magnetization measurements on single-crystal cubic SrCuTe$_2$O$_6$ with an applied magnetic field of along three inequivalent high symmetry directions $[100]$, $[110]$, and $[111]$ reveal weak magnetic anisotropy. The fits of the magnetic susceptibility to the result from a quantum Monte Carlo simulation on the Heisenberg spin-chain model, where the chain is formed via the dominant third-nearest-neighbor exchange interaction $J_3$, yield the intra-chain interaction $(J_3/k_B)$ between 50.12(7) K for the applied field along $[110]$ and 52.5(2) K along $[100]$ with about the same $g$-factor of 2.2. Single-crystal neutron diffraction unveils the transition to the magnetic ordered state as evidenced by the onset of the magnetic Bragg intensity at $T_textrm{N1}=5.25(9)$ K with no anomaly of the second transition at $T_textrm{N2}$ reported previously. Based on irreducible representation theory and magnetic space group analysis of powder and single-crystal neutron diffraction data, the magnetic structure in the Shubnikov space group $P4_132$, where the Cu$^{2+}$~$S=1/2$ spins antiferromagnetically align in the direction perpendicular to the spin chain, is proposed. The measured ordered moment of $0.52(6)~mu_B$, which represents 48% reduction from the expected value of $1~mu_B$, suggests the remaining influence of frustration resulting from the $J_1$ and $J_2$ bonds.
Dielectric and magnetic properties have been studied for poly-crystalline samples of quasi-one-dimensional frustrated spin-1/2 system Rb$_{2}$(Cu$_{1-x}$M$_{x}$)$_{2}$Mo$_{3}$O$_{12}$(M=Ni and Zn) which does not exhibit a three-dimensional magnetic transition due to quantum spin fluctuation and low dimensionality. A broad peak in the magnetic susceptibility - temperature curves originated from a short range helical ordering at low temperature is suppressed by the Ni and Zn substitution for Cu sites. The capacitance is found to anomalously increase with decreasing T below ~50 K, which is also suppressed by the impurity doping. The behavior of the anomalous capacitance component is found to be strongly connected with that of the magnetic susceptibility for Rb$_{2}$(Cu$_{1-x}$M$_{x}$)$_{2}$Mo$_{3}$O$_{12}$ which indicates that the low-temperature dielectric response is driven by the magnetism.
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