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Interactions among charge carriers in graphene can lead to the spontaneousbreaking of multiple degeneracies. When increasing the number of graphenelayers following rhombohedral stacking, the dominant role of Coulombinteractions becomes pronounced due to the significant reduction in kineticenergy. In this study, we employ phonon-polariton assisted near-field infraredimaging to determine the stacking orders of tetralayer graphene devices.Through quantum transport measurements, we observe a range of spontaneousbroken-symmetry states and their transitions, which can be finely tuned bycarrier density n and electric displacement field D. Specifically, we observe alayer antiferromagnetic insulator at n = D = 0 with a gap of approximately 15meV. Increasing D allows for a continuous phase transition from a layerantiferromagnetic insulator to a layer polarized insulator. By simultaneouslytuning n and D, we observe isospin polarized metals, includingspin-valley-polarized and spin-polarized metals. These transitions areassociated with changes in Fermi surface topology and are consistent with theStoner criteria. Our findings highlight the efficient fabrication of speciallystacked multilayer graphene devices and demonstrate that crystalline multilayergraphene is an ideal platform for investigating a wide range of brokensymmetries driven by Coulomb interactions.

Interaction-driven spontaneous broken-symmetry insulator and metals in ABCA tetralayer graphene