Interplay between adsorbed C60 fullerenes and point defects on a Si(111)3×3-In reconstructed surface

► Interplay between adsorbed C60 fullerenes and Si(111)3×3-In surface defects was detected. ► Substitutional Si-defects trap the fullerenes. ► Group of a few fullerenes can act as a trap for a mobile surface vacancy. ► Vacancy migration was detected using STM video observations. ► Pathways and energetics of vacancy motion were examined using DFT calculations.