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The pristine graphene is strongly diamagnetic. However, graphene with singlecarbon atom defects could exhibit paramagnetism with local magnetic moments ~1.5 per vacancy1-6. Theoretically, both the electrons and electrons of graphenecontribute to the magnetic moment of the defects, and the pi magnetism ischaracterizing of two spin-split DOS (density-of-states) peaks close to theDirac point1,6. Since its prediction, many experiments attempt to study this pimagnetism in graphene, whereas, only a notable resonance peak has been observedaround the atomic defects6-9, leaving the pi magnetism experimentally soelusive. Here, we report direct experimental evidence of the pi magnetism byusing scanning tunnelling microscope. We demonstrate that the localized stateof the atomic defects is split into two DOS peaks with energy separations ofseveral tens meV and the two spin-polarized states degenerate into a profoundpeak at positions with distance of ~ 1 nm away from the monovacancy. Strongmagnetic fields further increase the energy separations of the twospin-polarized peaks and lead to a Zeeman-like splitting. The effectiveg-factors geff around the atomic defect is measured to be about 40. Such agiant enhancement of the g-factor is attributed to the strong spin polarizationof electron density and large electron-electron interactions near the atomicvacancy.

Direct experimental evidence of pi magnetism of a single atomic vacancy in graphene