Anomalous spin relaxation in graphene nanostructures on the high temperature annealed surface of hydrogenated diamond nanoparticles.

The electronic and magnetic structures of diamond nanoparticles with a hydrogenated surface are investigated as a function of annealing temperature under vacuum annealing up to 800-1000 °C. Near edge X-ray absorption fine structure (NEXAFS) spectra together with elemental analysis show successive creation of defect-induced nonbonding surface states at the expense of surface-hydrogen atoms as the annealing temperature is increased above 800 °C. Magnetization and ESR spectra confirm the increase in the concentration of localized spins assigned to the nonbonding surface states upon the increase of the annealing temperature. Around 800 °C, surface defects collectively created upon the annealing result in the formation of graphene nano-islands which possess magnetic nonbonding edge states of π-electron origin. Interestingly, extremely slow spin relaxation is observed in the magnetization of the edge state spins at low temperatures. The relaxation time is well explained in terms of a lognormal distribution of magnetic anisotropy energies instead of the classical Néel relaxation mechanism with a unique magnetic anisotropy energy, in addition to the contribution of the quantum mechanical tunnelling mechanism. The spin-orbit interaction enhanced by the electrostatic potential gradient created at the interface between the core diamond particle and surface graphene nano-islands is responsible for the slow spin relaxation.