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The magnetic properties of carbon materials are at present the focus of intense research effort in physics, chemistry and materials science due to their potential applications in spintronics and quantum computing. Although the presence of spins in open-shell nanographenes has recently been confirmed, the ability to control magnetic coupling sign has remained elusive but highly desirable. Here, we demonstrate an effective approach of engineering magnetic ground states in atomically precise open-shell bipartite/nonbipartite nanographenes using combined scanning probe techniques and mean-field Hubbard model calculations. The magnetic coupling sign between two spins was controlled via breaking bipartite lattice symmetry of nanographenes. In addition, the exchange-interaction strength between two spins has been widely tuned by finely tailoring their spin density overlap, realizing a large exchange-interaction strength of 42 meV. Our demonstrated method provides ample opportunities for designer above-room-temperature magnetic phases and functionalities in graphene nanomaterials.

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The magnetization reversal induced by spin orbit torques in the presence of Dzyaloshinskii-Moriya interaction (DMI) in perpendicularly magnetized Ta/CoFeB/MgO structures were investigated by using a combination of Anomalous Hall effect measurement and Kerr effect microscopy techniques. By analyzing the in-plane field dependent spin torque efficiency measurements, an effective field value for the DMI of ~300 Oe was obtained, which plays a key role to stabilize Néel walls in the film stack. Kerr imaging reveals that the current-induced reversal under small and medium in-plane field was mediated by domain nucleation at the edge of the Hall bar, followed by asymmetric domain wall (DW) propagation. However, as the in-plane field strength increases, an isotropic DW expansion was observed before reaching complete reversal. Micromagnetic simulations of the DW structure in the CoFeB layer suggest that the DW configuration under the combined effect of the DMI and the external field is responsible for the various DW propagation behaviors.