Doublet-Singlet-Doublet Transition in a Single Organic Molecule Magnet On-Surface Constructed with up to 3 Aluminum Atoms

[Image: see text] Starting from a long aza-starphene neutral and nonmagnetic organic molecule, a single-molecule magnet is on-surface constructed using up to 3 light nonmagnetic aluminum (Al) atoms. Seldom observed in solution with transition-metal atoms and going from 1 to 3 Al coordinated atoms, the doublet-singlet-doublet transition is easily on-surface accessible using the scanning tunneling microscope single-atom and single-molecule manipulations on a gold(111) surface. With 3 coordinated Al atoms, the lateral vibration modes of the Al(3)-aza-starphene molecule magnet are largely frozen. Using the Kondo states, this opens the observation of the in-phase Al vertical atom vibrations and out-of-phase central phenyl vibrations.