Electrically controlled nonvolatile switching of single-atom magnetism in a Dy@C₈₄ single-molecule transistor

Single-atom magnetism switching is a key technique towards the ultimate data storage density of computer hard disks and has been conceptually realized by leveraging the spin bistability of a magnetic atom under a scanning tunnelling microscope. However, it has rarely been applied to solid-state transistors, an advancement that would be highly desirable for enabling various applications. Here, we demonstrate realization of the electrically controlled Zeeman effect in Dy@C₈₄ single-molecule transistors, thus revealing a transition in the magnetic moment from 3.8 μ_B to 5.1 μ_B for the ground-state G_N at an electric field strength of 3−10 MV/cm. The consequent magnetoresistance significantly increases from 600% to 1100% at the resonant tunneling point. Density functional theory calculations further corroborate our realization of nonvolatile switching of single-atom magnetism, and the switching stability emanates from an energy barrier of 92 meV for atomic relaxation. These results highlight the potential of using endohedral metallofullerenes for high-temperature, high-stability, high-speed, and compact single-atom magnetic data storage.