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We report that the {\pi}-electrons of graphene can be spin-polarized tocreate a phase with a significant spin-orbit gap at the Dirac point (DP) usinga graphene-interfaced topological insulator hybrid material. We have grownepitaxial Bi2Te2Se (BTS) films on a chemical vapor deposition (CVD) graphene.We observe two linear surface bands both from the CVD graphene notablyflattened and BTS coexisting with their DPs separated by 0.53 eV in thephotoemission data measured with synchrotron photons. We further demonstratethat the separation between the two DPs, {\Delta}D-D, can be artificiallyfine-tuned by adjusting the amount of Cs atoms adsorbed on the graphene to avalue as small as {\Delta}D-D = 0.12 eV to find any proximity effect induced bythe DPs. Our density functional theory calculation shows a spin-orbit gap of~20 meV in the {\pi}-band enhanced by three orders of magnitude from that of apristine graphene, and a concomitant phase transition from a semi-metallic to aquantum spin Hall phase when {\Delta}D-D $\leq$ 0.20 eV. We thus present apractical means of spin-polarizing the {\pi}-band of graphene, which can bepivotal to advance the graphene-based spintronics.

Proximity Effect Induced Electronic Properties of Epitaxial Graphene on Bi2Te2Se