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Second neighbor dominated exchange coupling in CaV4O9 has been obtained fromab initio density functional (DF) calculations. A DF-based self-consistentatomic deformation model reveals that the nearest neighbor coupling is smalldue to strong cancellation among the various superexchange processes. Exactdiagonalization of the predicted Heisenberg model yields spin-gap behavior ingood agreement with experiment. The model is refined by fitting to theexperimental susceptibility. The resulting model agrees very well with theexperimental susceptibility and triplet dispersion.Comment: 4 pages; 3 ps figures included in text; Revte

journal of the physical society of japan

AbInitioCalculation of Spin Gap Behavior in CaV4O9