Antiferromagnetic Dimers of Ni(II) in the S=1 Spin-Ladder Na₂Ni₂(C₂O₄)₃(H₂O)₂

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We report the synthesis, crystal structure and magnetic properties of the S=1 2-leg spin-ladder compound Na₂Ni₂(C₂O₄)₃(H₂O)₂. The magnetic properties were examined by magnetic susceptibility and pulsed high field magnetization measurements. The magnetic excitations have been measured in high field high frequency ESR. Although the Ni(II) ions form structurally a 2-leg ladder, an isolated dimer model consistently describes the observations very well. The analysis of the temperature dependent magnetization data leads to a magnetic exchange constant of J=43 K along the rungs of the ladder and an average value of the g-factor of 2.25. From the ESR measurements, we determined the single ion anisotropy to D=11.5 K. The validity of the isolated dimer model is supported by Quantum Monte Carlo calculations, performed for several ratios of interdimer and intradimer magnetic exchange and taking into account the experimentally determined single ion anisotropy. The results can be understood in terms of the different coordination and superexchange angles of the oxalate ligands along the rungs and legs of the 2-leg spin ladder.