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.
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