Tunable correlated states and spin-polarized phases in twisted bilayer–bilayer graphene

The recent discovery of correlated insulator states and superconductivity in magic-angle twisted bilayer graphene1,2 has enabled the experimental investigation of electronic correlations in tunable flat-band systems realized in twisted van der Waals heterostructures3–6. This novel twist angle degree of freedom and control should be generalizable to other two-dimensional systems, which may exhibit similar correlated physics behaviour, and could enable techniques to tune and control the strength of electron–electron interactions. Here we report a highly tunable correlated system based on small-angle twisted bilayer–bilayer graphene (TBBG), consisting of two rotated sheets of Bernal-stacked bilayer graphene. We find that TBBG exhibits a rich phase diagram, with tunable correlated insulator states that are highly sensitive to both the twist angle and the application of an electric displacement field, the latter reflecting the inherent polarizability of Bernal-stacked bilayer graphene7,8. The correlated insulator states can be switched on and off by the displacement field at all integer electron fillings of the moiré unit cell. The response of these correlated states to magnetic fields suggests evidence of spin-polarized ground states, in stark contrast to magic-angle twisted bilayer graphene. Furthermore, in the regime of lower twist angles, TBBG shows multiple sets of flat bands near charge neutrality, resulting in numerous correlated states corresponding to half-filling of each of these flat bands, all of which are tunable by the displacement field as well. Our results could enable the exploration of twist-angle- and electric-field-controlled correlated phases of matter in multi-flat-band twisted superlattices.