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Register a new userSinglet Ground State and Magnetization Plateaus in Ba$_3$Mn$_2$O$_8$
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Magnetic susceptibility and the magnetization process have been measured in green polycrystal. In this compound, the magnetic manganese ion exists as Mn$^{5+}$ in a tetrahedral environment, and thus the magnetic interaction can be described by an S=1 Heisenberg model. The ground state was found to be a spin singlet with an excitation gap $Delta/k_{rm B}=11.2$ K. Magnetization plateaus were observed at zero and at half of the saturation magnetization. These results indicate that the present system can be represented by a coupled antiferromagnetic dimer model.
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Strong spin-orbit coupling (SOC) effects of heavy $d$-orbital elements have long been neglected in describing the ground states of their compounds thereby overlooking a variety of fascinating and yet unexplored magnetic and electronic states, until recently. The spin-orbit entangled electrons in such compounds can get stabilized into unusual spin-orbit multiplet $J$-states which warrants severe investigations. Here we show using detailed magnetic and thermodynamic studies and theoretical calculations the ground state of Ba$_3$ZnIr$_2$O$_9$, a 6$H$ hexagonal perovskite is a close realisation of the elusive $J$~=~0 state. However, we find that local Ir moments are spontaneously generated due to the comparable energy scales of the singlet-triplet splitting driven by SOC and the superexchange interaction mediated by strong intra-dimer hopping. While the Ir ions within the structural Ir$_2$O$_9$ dimer prefers to form a spin-orbit singlet state (SOS) with no resultant moment, substantial interdimer exchange interactions from a frustrated lattice ensure quantum fluctuations till the lowest measured temperatures and stabilize a spin-orbital liquid phase.
We have measured the specific heat of the coupled spin-dimer antiferromagnet Ba$_3$Mn$_2$O$_8$ to 50 mK in temperature and to 29 T in the magnetic field. The experiment extends to the midpoint of the field region (25.9 T $leq H leq$ 32.3 T) of the magnetization plateau at 1/2 of the saturation magnetization, and reveals the presence of three ordered phases in the field region between that of the magnetization plateau and the low-field spin-liquid region. The exponent of the phase boundary with the thermally disordered region is smaller than the theoretical value based on the Bose-Einstein condensation of spin triplets. At zero field and 29 T, the specific-heat data show gapped behaviors characteristic of spin liquids. The zero-field data indicate that the gapped triplet excitations form two levels whose energies differ by nearly a factor of two. At least the lower level is well localized. The data at 29 T reveal that the low-lying excitations at the magnetization plateau are weakly delocalized.
We study the thermodynamic and high-magnetic-field properties of the magnetic insulator Ba$_5$CuIr$_3$O$_{12}$, which shows no magnetic order down to 2 K consistent with a spin liquid ground state. While the temperature dependence of the magnetic susceptibility and the specific heat shows only weak antiferromagnetic correlations, we find that the magnetization does not saturate up to a field of 59 Tesla, leading to an apparent contradiction. We demonstrate that the paradox can be resolved, and all of the experimental data can be consistently described within the framework of random singlet states. We demonstrate a generic procedure to derive the exchange coupling distribution $P(J)$ from the magnetization measurements and use it to show that the experimental data is consistent with the power-law form $P(J)sim J^{-alpha}$ with $alpha approx 0.6 $. Thus, we reveal that high-magnetic-field measurements can be essential to discern quantum spin liquid candidates from disorder dominated states that do not exhibit long-range order.
In an ideal classical pyrochlore antiferromagnet without perturbations, an infinite degeneracy at a ground state leads to absence of a magnetic order and spin-glass transition. Here we present Na$_3$Mn(CO$_3$)$_2$Cl as a new candidate compound where classical spins are coupled antiferromagnetically on the pyrochlore lattice, and report its structural and magnetic properties.The temperature dependences of the magnetic susceptibility and heat capacity, and the magnetization curve are consistent with those of an $S$ = 5/2 pyrochlore lattice antiferromagnet with nearest-neighbor interactions of 2 K. Neither an apparent signature of a spin-glass transition nor a magnetic order is detected in magnetization and heat capacity measurements, or powder neutron diffraction experiments. On the other hand, an antiferromagnetic short-range order from the nearest neighbors is evidenced by the $Q$-dependence of the diffuse scattering which develops around 0.85 AA$^{-1}$. A high degeneracy near the ground state in Na$_3$Mn(CO$_3$)$_2$Cl is supported by the magnetic entropy estimated as almost 4 J K$^{-2}$ mol$^{-1}$ at 0.5 K.
We study low energy excitations in the quantum breathing pyrochlore antiferromagnet Ba$_3$Yb$_2$Zn$_5$O$_{11}$ by combination of inelastic neutron scattering (INS) and thermodynamical properties measurements. The INS spectra are quantitatively explained by spin-1/2 single-tetrahedron model having $XXZ$ anisotropy and Dzyaloshinskii-Moriya interaction. This model has a two-fold degeneracy of the lowest-energy state per tetrahedron and well reproduces the magnetization curve at 0.5 K and heat capacity above 1.5 K. At lower temperatures, however, we observe a broad maximum in the heat capacity around 63 mK, demonstrating that a unique quantum ground state is selected due to extra perturbations with energy scale smaller than the instrumental resolution of INS.
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