Ferromagnetic stability optimization via oxygen-vacancy control in single-atom Co/TiO nanostructures.

Oxygen vacancies and their correlation with the nanomagnetism and electronic structure are crucial for applications in dilute magnetic semiconductors design applications. Here, we report on cobalt single atom-incorporated titanium dioxide (TiO) monodispersed nanoparticles synthesized using a thermodynamic redistribution strategy. Using advanced synchrotron-based X-ray techniques and simulations, we find trivalent titanium is absent, indicating trivalent cations do not influence ferromagnetic (FM) stability. Density functional theory calculations show that the FM stability between Co ions is very weak. However, electron doping from additional oxygen vacancies can significantly enhance this FM stability, which explains the observed room-temperature ferromagnetism. Moreover, our calculations illustrate enhanced FM interactions between Co + V complexes with additional oxygen vacancies. This study explores the electronic structure and room-temperature ferromagnetism using monodispersed nanocrystallites with single-atom-incorporated TiO nanostructures. The strategies described herein offer promise in revealing magnetism in other single-atom-incorporated nanostructures.