Abstract Utilising the CALYPSO code and DFT calculations, the systematic exploration of the structural, electronic, and magnetic properties of titanium-doped magnesium clusters, Ti2Mgn (n = 1–11), was carried out. The findings show that Ti2Mgn clusters undergo a structural transformation from 2D to 3D when n equals 2. From n = 6, the octahedral geometries serve as fundamental building blocks for subsequent structures except for Ti2Mg8, giving rise to numerous derivative Ti2Mgn clusters.
