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We report the complex magnetic phase diagram and electronic structure ofCr2(Te1-xWx)O6 systems. While compounds with different x values possess thesame crystal structure, they display different magnetic structures below andabove xc = 0.7, where both the transition temperature TN and sublatticemagnetization (Ms) reach a minimum. Unlike many known cases where magneticinteractions are controlled either by injection of charge carriers or bystructural distortion induced via chemical doping, in the present case it isachieved by tuning the orbital hybridization between Cr 3d and O 2p orbitalsthrough W 5d states. The result is supported by ab-initio electronic structurecalculations. Through this concept, we introduce a new approach to tunemagnetic and electronic properties via chemical doping.

Tuning the magnetic exchange via a control of orbital hybridization in Cr2(Te1-xWx)O6