As liquids crystallize into solids on cooling, spins in magnets generally form periodic order. However, three decades ago, it was theoretically proposed that spins on a triangular lattice form a liquidlike disordered state at low temperatures. Whether or not a spin liquid is stabilized by geometrical frustration has remained an active point of inquiry ever since. Our thermodynamic and neutron measurements on NiGa2S4, a rare example of a two-dimensional triangular lattice antiferromagnet, demonstrate that geometrical frustration stabilizes a low-temperature spin-disordered state with coherence beyond the two-spin correlation length. Spin liquid formation may be an origin of such behavior.

Strongly frustrated magnetism of the metallic pyrochlore oxide Pr2Ir2O7 has been revealed by single crystal study. While Pr 4f moments have an antiferromagnetic RKKY interaction energy scale of /T*/ = 20 K mediated by Ir 5d-conduction electrons, no magnetic long-range order is found except for partial spin freezing at 120 mK. Instead, the Kondo effect, including a lnT dependence in the resistivity, emerges and leads to a partial screening of the moments below /T*/. Our results indicate that the underscreened moments show spin-liquid behavior below a renormalized correlation scale of 1.7 K.

We have revealed the phase diagram of Ca2-xSrxRuO4: the quasi-two-dimensional Mott transition system that connects the Mott insulator Ca2RuO4 with the spin-triplet superconductor Sr2RuO4. Adjacent to the metal/nonmetal transition at x approximately 0.2, we found an antiferromagnetically correlated metallic region where non-Fermi-liquid behavior in resistivity is observed. Besides this, the critical enhancement of susceptibility toward the region boundary at x(c) approximately 0.5 suggests the crossover of magnetic correlation to a nearly ferromagnetic state, which evolves into the spin-triplet superconductor Sr2RuO4.

The crystal and magnetic structure of Ca 2 RuO 4 ͑CRO͒ has been studied by powder neutron diffraction. CRO was synthesized in two different modifications ͑stoichiometric and containing excess oxygen͒ whose crystal structures are, in spite of strong differences in the lattice constants, closely related. Both structures are derived from the ideal K 2 NiF 4 structure type by a rotation of the RuO 6 octahedra around the long axis, combined with a tilt around an axis lying in the RuO 2 plane. The orientation of the tilt axis seems to distinguish the two room-temperature symmetries; the excess oygen compound is characterized by a smaller tilt angle and shorter Ru-O in-plane bond distances. Stoichiometric CRO undergoes large structural changes on cooling, though no symmetry change was detected. In contrast, the excess oxygen containing compound undergoes a first-order structural phase transition accompanied by a change from metallic to insulating behavior in the electric resistivity. Both compounds exhibit antiferromagnetic order below 110-150 K; for the stoichiometric sample, the onset of magnetic order is associated with several structural anomalies.

The phase diagram of Ca 2−x Sr x RuO 4 has been studied by neutron diffraction on powder and single-crystalline samples. The experiments reveal antiferromagnetic order and structural distortions characterized by tilts and rotations of the RuO6-octahedra. There is strong evidence that the structural details of the isovalent samples tune the magnetic as well as the electronic behavior. In particular we observe for low Sr-concentration a metal insulator transition associated with a structural change and magnetic ordering.