Alkali effects on the electronic states of K3C60 and Rb3C60

The electronic states in metallic alkali fullerides K₃C₆₀ and Rb₃C₆₀, are studied in detail by cw- and pulsed-ESR. The ESR linewidth associated with conduction electrons varies substantially, depending sensitively on the alkali metals used. It is clearly revealed that the linewidth is homogeneous and is strongly controlled by the spin-lattice relaxation times (T₁) determined via the spin-orbit interactions of the small fraction of s electrons remaining on the alkali atoms. The results indicate that the electron transfer from the alkali atoms to C₆₀ is not perfectly complete, with the remaining fraction being much greater in the tetrahedral sites than in the octahedral sites of the face-centered cubic lattice.