Optically Controlled Molecular Metallofullerene Magnetism via an Azobenzene-Functionalized Metal–Organic Framework

Molecular magnets with optically controlled property have significant applications in data storage and quantum information processing. Herein, we report the optically controlled molecular magnetism of endohedral metallofullerenes, Sc3C2@C80 and DySc2N@C80, by incarcerating them into the pores of a photoswitchable azobenzene-functionalized metal–organic framework (MOF) (AzoMOF). After ultraviolet (365 nm) irradiation, the isomerization of azobenzene groups in the AzoMOF was found to be able to modulate the spin relaxation of Sc3C2@C80 and also improve the single-molecule magnet behavior of DySc2N@C80. The photoisomerization of azobenzene side groups changes the host–guest interaction between metallofullerene and AzoMOF pores and endows them with the potential to modulate the magnetic properties with light. These findings offer an effective method to create smart molecular magnetic materials and also promote their applications in information recording, spintronics, and sensors.