Spatially Resolving Electron Spin Resonance of π-Radical in Single-molecule Magnet

The spintronic properties of magnetic molecules have attracted significant scientific attention. Special emphasis has been placed on the qubit for quantum information processing. The single molecule magnet, bis(phthalocyaninato (Pc)) Tb(III) (TbPc2), is one of the best examined cases in which the delocalized π-radical electron spin of the Pc ligand plays the key role in reading and intermediating the localized Tb spin qubits. We utilized the electron spin resonance (ESR) technique implemented on scanning tunneling microscope (STM) and use it to measure local ESR of single TbPc2 molecule decoupled from the Cu(100) substrate by 2 monolayers NaCl film to identify the π-radical spin. We detected the ESR signal at the ligand positions at the resonance condition expected for the S = 1/2 spin. The results reveal that the π-radical electron is delocalized within the ligands and exhibits intramolecular coupling susceptible to the chemical environment.