Evidence for the singlet-dimer ground state in an S = 1 antiferromagnetic bond alternating chain

Susceptibility, ESR, and magnetization measurements have been performed on single crystals of an S = 1 bond alternating chain compound: [Ni(333-tet) (mu-NO2)] (ClO4) (333-tet = N,N'-bis(3-aminopropyl)propane-1,3-diamine) and the compound doped with a small amount of Zn. We observed an anomalous angular dependence in the Zn-doped sample. These results are well explained by the model based on the valence-bond solid picture for the singlet-dimer phase. The picture implies that the free spins of S = 1 with a positive uniaxial single-ion anisotropy are induced at the edges of the chains without forming the singlet dimer.