  We report the complex magnetic phase diagram and electronic structure of
Cr2(Te1-xWx)O6 systems. While compounds with different x values possess the
same crystal structure, they display different magnetic structures below and
above xc = 0.7, where both the transition temperature TN and sublattice
magnetization (Ms) reach a minimum. Unlike many known cases where magnetic
interactions are controlled either by injection of charge carriers or by
structural distortion induced via chemical doping, in the present case it is
achieved by tuning the orbital hybridization between Cr 3d and O 2p orbitals
through W 5d states. The result is supported by ab-initio electronic structure
calculations. Through this concept, we introduce a new approach to tune
magnetic and electronic properties via chemical doping.
