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In the fundamental understanding of magnetic interactions between atoms in solids, the crystal lattice is one of the key parameters. As the effective tool for controlling the lattice using tensile stress is limited, there are only few demonstrations of the control in magnetic properties with expanding the lattice structure. Here, we observe that the Curie temperature (Tc) of quasi two-dimensional Cr2Ge2Te6 with NiO overlayer doubles from ~60 K to ~120 K, describe a clear correlation of magnetic properties with lattice expansion, which is characterized by several probes and computational approaches, and address on the mechanisms leading to the increase in Tc via the change in exchange interactions.

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