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Spin-polarized two-dimensional materials with large and tunablespin-splitting energy promise the field of 2D spintronics. While graphene hasbeen a canonical 2D material, its spin properties and tunability are limited.Here, we demonstrate the emergence of robust spin-polarization in graphene withlarge and tunable spin-splitting energy of up to 132 meV at zero appliedmagnetic fields. The spin polarization is induced through a magnetic exchangeinteraction between graphene and the underlying ferrimagnetic oxide insulatinglayer, Tm3Fe5O12, as confirmed by its X-ray magnetic circular dichroism. Thespin-splitting energies are directly measured and visualized by the shift intheir landau fan diagram mapped by analyzing the measured subnikov-de-Haasoscillations as a function of applied electric fields, showing consistent fitwith our first-principles and machine learning calculations. Further, theobserved spin-splitting energies can be tuned over a broad range between 98 and166 meV by cooling fields. Our methods and results are applicable to othertwo-dimensional (magnetic) materials and heterostructures, and offer greatpotential for developing next-generation spin logic and memory devices.

Direct Determination of Spin-Splitting Energy in Magnetic Graphene by Landau Fan Shifts