Antiferromagnetically coupled S=1/2 spins on an isotropic triangular lattice is the paradigm of frustrated quantum magnetism, but structurally ideal realizations are rare. Here we investigate NaYbO2, which hosts an ideal triangular lattice of Jeff=1/2 moments with no inherent site disorder. No signatures of conventional magnetic order appear down to 50 mK, strongly suggesting a quantum spin liquid ground state. We observe a two-peak specific heat and a nearly quadratic temperature dependence in accord with expectations for a two-dimensional Dirac spin liquid. Application of a magnetic field strongly perturbs the quantum disordered ground state and induces a clear transition into a collinear ordered state consistent with a long-predicted "up-up-down" structure for a triangular lattice XXZ Hamiltonian driven by quantum fluctuations. The observation of spin liquid signatures in zero field and quantum-induced ordering in intermediate fields in the same compound demonstrate an intrinsically quantum disordered ground state. We conclude that NaYbO2 is a model, versatile platform for exploring spin liquid physics with full tunability of field and temperature.Exotic ground states of quantum antiferromagnets are encouraged by the combination of low dimensionality, geometric frustration, and inherent anisotropies. Planar triangular lattices have long been sought as platforms for stabilizing them 1-7 ; however, ideal manifestations that do not break crystallographic or exchange symmetries upon approaching the quantum regime are rare. The organic compounds κ-(BEDT-TTF)2Cu2(CN)3 8 and EtMe3Sb[Pd(dmit)2]2 9 are two promising examples of triangular lattices with S=1/2 moments and a dynamically disordered spin ground state. However, S=1/2 inorganic analogs such as Ba3CoSb2O9 10 , Ba8CoNb6O24 11 , and NaTiO2 12-14 either order magnetically or undergo a lattice deformation and dimerization upon cooling. A key roadblock in inorganic systems is the identification of a material with a high crystallographic symmetry, rigid structure, and minimal defect mechanisms that also contains magnetic ions possessing strong quantum fluctuations. Ideally, the magnetic ions should be located at high symmetry positions that preclude antisymmetric Dzyaloshinskii-Moriya exchange from lifting geometric frustration at low temperatures.As an alternative to S=1/2 based compounds, rare earth ions with ground state doublets may also engender enhanced quantum fluctuations when decorating a triangular lattice. Specifically, recent studies have shown that the spin-orbit entangled Jeff=1/2 moments of Yb 3+ ions on this lattice may exhibit a variety of nearly degenerate magnetic states 15-22 . Given the appropriate anisotropies and when driven close
We present results from muon spin relaxation/rotation, magnetization, neutron scattering, and transport measurements on polycrystalline samples of the pyrochlore iridates Y 2 Ir 2 O 7 (Y-227) and Yb 2 Ir 2 O 7 (Yb-227). Well-defined spontaneous oscillations of the muon asymmetry are observed together with hysteretic behavior in magnetization below 130 K in Yb-227, indicative of commensurate long-range magnetic order. Similar oscillations are observed in Y-227 below 150 K; however, the onset of hysteretic magnetization at T = 190 K indicates a transition to an intermediate state lacking long-range order as observed in Nd-227. Our results also show that insulating members of the iridate family have nearly identical magnetic ground states, and that the presence of magnetic A-site species does not play any significant role in altering the ground-state properties.
The experimental and theoretical study of the electron spin dynamics in the anionic form of a single-ion molecule magnet (SIMM), the bis-phthalocyaninato terbium (III) molecule [Pc(2)Tb](-)[TBA](+), has been addressed by means of solid state (1)H NMR spectroscopy. The magnetic properties of the caged Tb(3+) metal center were investigated in a series of diamagnetically diluted preparations, where the excess of tetrabutylamonium bromide ([TBA]Br)(n) salt was used as diamagnetic matrix complement. We found that a high temperature activated spin dynamics characterizes the systems, which involved phonon-assisted transitions among the crystal field levels in qualitative agreements with literature results. However, the activation barriers in these processes range from 641 cm(-1) for the diamagnetically diluted samples to 584 cm(-1) for those undiluted; thus, they exhibit barriers 2-3 times larger than witnessed in earlier (230 cm(-1)) reports (e.g., Ishikawa, N.; Sugita, M.; Ishikawa, T.; Koshihara, S.; Kaizu, Y. J. Am. Chem. Soc. 2003, 125, 8694-8695). At cryogenic temperatures, fluctuations are driven by tunneling processes between the m = +6 and -6 low-energy levels. We found that the barrier Delta and the tunneling rates change from sample to sample and especially the diamagnetically diluted [Pc(2)Tb](-) molecules appear affected by the sample's magneto/thermal history. These observations emphasize that matrix arrangements around [Pc(2)Tb](-) can appreciably alter the splitting of the crystal field levels, its symmetry, and hence, the spin dynamics. Therefore, understanding how small differences in molecular surroundings (as for instance occurring by depositing on surfaces) can trigger substantial modifications in the SIMM property is of utmost importance for the effective operation of such molecules for single-molecule data storage, for example.
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