Intracage vibrations and Zeeman effect in Y3N@C80 single-molecule transistors

Clusterfullerenes, which contain a cluster rather than single-atom inclusions, exhibit more complex internal structures and greater degrees of freedom for motion. Trimetallic nitride clusterfullerenes have attracted significant attention due to their diversity and potential applications, among which Y3N@C80 stands out for its charge-transfer characteristics in electronic excitations, owing to the unique distribution of molecular orbitals near the Fermi level. Here, we have fabricated single-molecule transistor devices using Y3N@C80. Transport measurements at liquid helium temperature revealed a series of excited state energy levels, which were matched to corresponding vibrational modes through comparison with Raman spectra and density functional theory calculations. Additionally, we measured charge-state-dependent magnetic responses, revealing the electron and spin-filling patterns of the molecular orbitals in Y3N@C80. These results enhance our understanding of the dynamics and molecular spin–orbit characteristics of clusterfullerenes, indicating their potential for multifunctional applications.