Variety of valence bond states formed of frustrated spins on triangular lattices based on a two-level system Pd(dmit)2.

Recent studies on the physical properties of the triangular system based on the Pd(dmit)2 salts (dmit=1,3-dithiole-2-thione-4,5-dithiolate) are reviewed. Quantum chemical architectures of the Pd(dmit)2 molecule and its dimer are introduced with emphasis on the strong dimerization of a two-level system, which provides unique physical properties of the salts. The magnetic properties are outlined in view of the magneto-structural correlation specific to the frustrated spin systems. Some newly discovered ground states and their origins are discussed, for which the valence bond formation plays a key role. Among them, the two-level structure is crucial for the novel charge-separated state found in two salts. The valence bond ordering, similar to the spin-Peierls transition, has been found in a two-dimensional frustrated spin system. The physical aspects and possible relation to the pressure-induced superconductivity are discussed.