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The structural, transport, magnetic and optical properties of the double perovskite A2CrWO6 with A = Sr, Ba, Ca have been studied. By varying the alkaline earth ion on the A site, the influence of steric effects on the Curie temperature TC and the saturation magnetization has been determined. A maximum TC = 458 K was found for Sr2CrWO6 having an almost undistorted perovskite structure with a tolerance factor f ≃ 1. For Ca2CrWO6 and Ba2CrWO6 structural changes result in a strong reduction of TC. Our study strongly suggests that for the double perovskites in general an optimum TC is achieved only for f ≃ 1, that is, for an undistorted perovskite structure. Electron doping in Sr2CrWO6 by a partial substitution of Sr 2+ by La 3+ was found to reduce both TC and the saturation magnetization Ms. The reduction of Ms could be attributed both to band structure effects and the Cr/W antisites induced by doping. Band structure calculations for Sr2CrWO6 predict an energy gap in the spin-up band, but a finite density of states for the spin-down band. The predictions of the band structure calculation are consistent with our optical measurements. Our experimental results support the presence of a kinetic energy driven mechanism in A2CrWO6, where ferromagnetism is stabilized by a hybridization of states of the nonmagnetic W-site positioned in between the high spin Cr-sites.

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