We consider theoretically the influence of crystalline fields on the electronic structure of graphene placed on a layered material with reduced symmetry and large spin-orbit coupling (SOC). We use a perturbative procedure combined with the Slater-Koster method to derive the low-energy effective Hamiltonian around the $K$ points and estimate the magnitude of the effective couplings. Two simple models for the envisaged graphene-substrate hybrid bilayer are considered, in which the relevant atomic orbitals hybridize with either top or hollow sites of the graphene honeycomb lattice. In both cases, the interlayer coupling to a crystal-field-split substrate is found to generate highly anisotropic proximity spin-orbit interactions, including in-plane spin-valley coupling. Interestingly, when an anisotropic intrinsic-type SOC becomes sizeable, the bilayer system is effectively a quantum spin Hall insulator characterized by in-plane helical edge states robust against Bychkov-Rashba effect. Finally, we discuss the type of substrate required to achieve anisotropic proximity-induced SOC and suggest possible candidates to further explore crystal field effects in graphene-based heterostructures.
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