Structural and doping effects in the half-metallic double perovskite $A_2$CrWO$_6$

he structural, transport, magnetic and optical properties of the double perovskite $A_2$CrWO$_6$ with $A=\text{Sr, Ba, Ca}$ have been studied. By varying the alkaline earth ion on the $A$ site, the influence of steric effects on the Curie temperature $T_C$ and the saturation magnetization has been determined. A maximum $T_C=458$ K was found for Sr$_2$CrWO$_6$ having an almost undistorted perovskite structure with a tolerance factor $f\simeq 1$. For Ca$_2$CrWO$_6$ and Ba$_2$CrWO$_6$ structural changes result in a strong reduction of $T_C$. Our study strongly suggests that for the double perovskites in general an optimum $T_C$ is achieved only for $f \simeq 1$, that is, for an undistorted perovskite structure. Electron doping in Sr$_2$CrWO$_6$ by a partial substitution of Sr$^{2+}$ by La$^{3+}$ was found to reduce both $T_C$ and the saturation magnetization $M_s$. The reduction of $M_s$ could be attributed both to band structure effects and the Cr/W antisites induced by doping. Band structure calculations for Sr$_2$CrWO$_6$ 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 $A_2$CrWO$_6$, where ferromagnetism is stabilized by a hybridization of states of the nonmagnetic W-site positioned in between the high spin Cr-sites.