Electron spin spectroscopy of single TEMPO dimers coupled via interfering tunneling currents

Abstract: We report the detection of electron spin resonance (ESR) in individual dimers of the stable free radical 2,2,6,6-tetramethyl-piperidine-1-oxyl (TEMPO). ESR is measured by the current fluctuations in a scanning tunnelling microscope (ESR-STM method). The multi-peak power spectra, distinct from macroscopic data, are assigned to dimers having exchange and Dzyaloshinskii-Moriya interactions in presence of spin-orbit coupling. These interactions are generated in our model by interfering electronic tunneling pathways from tip to sample via the dimer's two molecules. This is the first demonstration that tunneling via two spins is a valid mechanism of the ESR-STM method.