Electron Spin Manipulation via Encaged Cluster: Differing Anion Radicals of Y2@C82-Cs, Y2C2@C82-Cs, and Sc2C2@C82-Cs

Endohedral metallofullerene species with controllable electron spin have attracted increasing attention along with their potential application in quantum information processing. In this paper, we report the electron spin manipulation via encage cluster through comparative studies on the anion radicals of metallofullerene Y2@C82-Cs, Y2C2@C82-Cs, and Sc2C2@C82-Cs. Although these three radical species have the same parent fullerene cage, we found that the unpaired spin characteristics as well as metal-spin couplings of them can be greatly affected by endohedral clusters. Furthermore, based on theoretical calculations, it was revealed that the encaged clusters can affect the electronic population of pristine endohedral metallofullerenes and eventually manipulate the spin distribution of their corresponding anion radicals. Our findings are referential to the spin coherence in information processing due to the variable paramagnetism of these metallofullerene radicals.