Van der Waals heterostructures provide a rich platform for emergent physics due to their tunable hybridization of electronic orbital- and spin-degrees of freedom. Here, we show that a heterostructure formed by twisted bilayer graphene sandwiched between ferromagnetic insulators develops flat bands stemming from the interplay between twist, exchange proximity and spin-orbit coupling. We demonstrate that in this flat-band regime, the spin degree of freedom is hybridized, giving rise to an effective triangular superlattice with valley as a degenerate pseudospin degree of freedom. Incorporating electronic interactions at half-filling leads to a spontaneous valley-mixed state, i.e., a correlated state in the valley sector with geometric frustration of the valley spinor. We show that an electric interlayer bias generates an artificial valley-orbit coupling in the effective model, controlling both the valley anisotropy and the microscopic details of the correlated state, with both phenomena understood in terms of a valley-Heisenberg model with easy-plane anisotropic exchange. Our results put forward twisted graphene encapsulated between magnetic van der Waals heterostructures as platforms to explore purely valley-correlated states in graphene.
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